Lube oil-dependent ash chemistry on soot oxidation reactivity in a gasoline direct-injection engine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Choi, Seungmok; Seong, Heeje

Gasoline particulate filters (GPF) are considered an enabling technology to meet stringent particulate matter (PM) regulations for gasoline direct-injection (GDI) engines, which are known to produce significant PM emissions. While ash loading in filters has been recognized to be detrimental in filter performance by increasing back pressure, increased ash fractions in soot were observed to enhance soot oxidation. In this study, GDI soot samples derived from different gasoline/lube oil blends were evaluated to identify potential promoting factors when formulated lube oils were dosed into gasoline fuel. Ca-derived ash enhanced soot oxidation remarkably, while P- and ZDDP-derived ash deteriorated soot oxidation.more » It is apparent that the promoting effect of lube oil-derived ash is due mainly to the Ca component that is the most abundant among additive components in lube oil. Bulk and surface analyses of these ash compounds indicate that Ca-derived ash would be complex compounds, while the contribution of CaSO 4, which is one of the most abundant ash compounds from diesel engines, is almost negligible. For the validation of the ash promoting impact in filters, the regeneration experiments were compared for a TWC-coated GPF in a GDI engine before and after ash loading was performed. The pressure drop of the ash-loaded GPF decreased noticeably in the initial regeneration stage and it increased gradually, whereas that of no ash-loaded GPF increased gradually without any reduction. So, it is concluded that the ash layer in the GPF assisted soot oxidation in the early regeneration stage when it was in close contact with soot.« less

First in-flight synchrotron X-ray absorption and photoemission study of carbon soot nanoparticles.

PubMed

Ouf, F-X; Parent, P; Laffon, C; Marhaba, I; Ferry, D; Marcillaud, B; Antonsson, E; Benkoula, S; Liu, X-J; Nicolas, C; Robert, E; Patanen, M; Barreda, F-A; Sublemontier, O; Coppalle, A; Yon, J; Miserque, F; Mostefaoui, T; Regier, T Z; Mitchell, J-B A; Miron, C

2016-11-24

Many studies have been conducted on the environmental impacts of combustion generated aerosols. Due to their complex composition and morphology, their chemical reactivity is not well understood and new developments of analysis methods are needed. We report the first demonstration of in-flight X-ray based characterizations of freshly emitted soot particles, which is of paramount importance for understanding the role of one of the main anthropogenic particulate contributors to global climate change. Soot particles, produced by a burner for several air-to-fuel ratios, were injected through an aerodynamic lens, focusing them to a region where they interacted with synchrotron radiation. X-ray photoelectron spectroscopy and carbon K-edge near-edge X-ray absorption spectroscopy were performed and compared to those obtained for supported samples. A good agreement is found between these samples, although slight oxidation is observed for supported samples. Our experiments demonstrate that NEXAFS characterization of supported samples provides relevant information on soot composition, with limited effects of contamination or ageing under ambient storage conditions. The highly surface sensitive XPS experiments of airborne soot indicate that the oxidation is different at the surface as compared to the bulk probed by NEXAFS. We also report changes in soot's work function obtained at different combustion conditions.

Burners and combustion apparatus for carbon nanomaterial production

DOEpatents

Alford, J. Michael; Diener, Michael D; Nabity, James; Karpuk, Michael

2013-02-05

The invention provides improved burners, combustion apparatus, and methods for carbon nanomaterial production. The burners of the invention provide sooting flames of fuel and oxidizing gases. The condensable products of combustion produced by the burners of this invention produce carbon nanomaterials including without limitation, soot, fullerenic soot, and fullerenes. The burners of the invention do not require premixing of the fuel and oxidizing gases and are suitable for use with low vapor pressure fuels such as those containing substantial amounts of polyaromatic hydrocarbons. The burners of the invention can operate with a hot (e.g., uncooled) burner surface and require little, if any, cooling or other forms of heat sinking. The burners of the invention comprise one or more refractory elements forming the outlet of the burner at which a flame can be established. The burners of the invention provide for improved flame stability, can be employed with a wider range of fuel/oxidizer (e.g., air) ratios and a wider range of gas velocities, and are generally more efficient than burners using water-cooled metal burner plates. The burners of the invention can also be operated to reduce the formation of undesirable soot deposits on the burner and on surfaces downstream of the burner.

Burners and combustion apparatus for carbon nanomaterial production

DOEpatents

Alford, J. Michael; Diener, Michael D.; Nabity, James; Karpuk, Michael

2007-10-09

The invention provides improved burners, combustion apparatus, and methods for carbon nanomaterial production. The burners of the invention provide sooting flames of fuel and oxidizing gases. The condensable products of combustion produced by the burners of this invention produce carbon nanomaterials including without limitation, soot, fullerenic soot, and fullerenes. The burners of the invention do not require premixing of the fuel and oxidizing gases and are suitable for use with low vapor pressure fuels such as those containing substantial amounts of polyaromatic hydrocarbons. The burners of the invention can operate with a hot (e.g., uncooled) burner surface and require little, if any, cooling or other forms of heat sinking. The burners of the invention comprise one or more refractory elements forming the outlet of the burner at which a flame can be established. The burners of the invention provide for improved flame stability, can be employed with a wider range of fuel/oxidizer (e.g., air) ratios and a wider range of gas velocities, and are generally more efficient than burners using water-cooled metal burner plates. The burners of the invention can also be operated to reduce the formation of undesirable soot deposits on the burner and on surfaces downstream of the burner.

Spectroscopic and solubility characteristics of oxidized soots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chughtai, A.R.; Jassim, J.A.; Peterson, J.H.

1991-01-01

Spectroscopic and solubility studies of reaction products of soot (black carbon) with O{sub 3}, NO{sub 2}/N{sub 2}O{sub 4}, and SO{sub 2} have revealed a relationship between reactivity and product solubility and structure. A remarkably high solubility of ozonated n-hexane soot has its origin in the formation of anhydride and lactone surface structures and their subsequent hydrolysis to carboxylic acid species. Calculations indicate that the rate of surface carboxylation of 0.1-{mu}m diameter spheroidal soot particles, in the presence of 50 ppbv ozone at ambient temperature, is such that solubilization may occur within a 30-minute time frame. Measurements on ambient air aerosolmore » samples in metropolitan Denver are consistent with these observations and demonstrate the high reactivity of soot with ozone even at very low levels in natural systems.« less

Oxidation characteristics of gasoline direct-injection (GDI) engine soot: Catalytic effects of ash and modified kinetic correlation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Choi, Seungmok; Seong, Heeje

In this paper, experimental analyses are conducted into the GDI soot oxidation characteristics as dependent on engine operating conditions. Soot is sampled at various engine operating conditions of a commercial 2.4 L GDI engine with a naturally aspirated, homogeneous, and stoichiometric operation strategy. The oxidation reactivity, ash composition, and carbon nanostructure of the GDI soot samples are analyzed using thermogravimetric analysis (TGA), scanning electron microscope–energy-dispersive spectroscopy (SEM-EDS), high-resolution transmission electron microscopy (HR-TEM), and Raman spectroscopy. Based on the analyses, a global GDI soot oxidation mechanism is proposed which includes the effects of soluble organic fractions (SOF)/weakly bonded carbon (WBC), andmore » three types of ash on GDI soot oxidation. The results show that GDI soot contains an order of magnitude higher ash fraction than does conventional diesel soot, and oxidation reactivity is significantly enhanced by the catalytic effects of ash, as a function of ash content in soot. A modified empirical kinetic correlation for GDI soot oxidation is suggested on the basis of the results, and the modified kinetic correlation predicts the GDI soot oxidation rate accurately for various engine operation points at wide ranges of soot conversion and temperature without modifying kinetic parameters. The kinetic parameters are determined from isothermal and non-isothermal thremogravimetric analysis (TGA) soot oxidation tests; the methods are elucidated in detail.« less

Oxidation characteristics of gasoline direct-injection (GDI) engine soot: Catalytic effects of ash and modified kinetic correlation

DOE PAGES

Choi, Seungmok; Seong, Heeje

2015-03-02

In this paper, experimental analyses are conducted into the GDI soot oxidation characteristics as dependent on engine operating conditions. Soot is sampled at various engine operating conditions of a commercial 2.4 L GDI engine with a naturally aspirated, homogeneous, and stoichiometric operation strategy. The oxidation reactivity, ash composition, and carbon nanostructure of the GDI soot samples are analyzed using thermogravimetric analysis (TGA), scanning electron microscope–energy-dispersive spectroscopy (SEM-EDS), high-resolution transmission electron microscopy (HR-TEM), and Raman spectroscopy. Based on the analyses, a global GDI soot oxidation mechanism is proposed which includes the effects of soluble organic fractions (SOF)/weakly bonded carbon (WBC), andmore » three types of ash on GDI soot oxidation. The results show that GDI soot contains an order of magnitude higher ash fraction than does conventional diesel soot, and oxidation reactivity is significantly enhanced by the catalytic effects of ash, as a function of ash content in soot. A modified empirical kinetic correlation for GDI soot oxidation is suggested on the basis of the results, and the modified kinetic correlation predicts the GDI soot oxidation rate accurately for various engine operation points at wide ranges of soot conversion and temperature without modifying kinetic parameters. The kinetic parameters are determined from isothermal and non-isothermal thremogravimetric analysis (TGA) soot oxidation tests; the methods are elucidated in detail.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Howard, J. B.; Richter, H.

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 whilemore » 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.« less

Black carbon surface oxidation and organic composition of beech-wood soot aerosols

NASA Astrophysics Data System (ADS)

Corbin, J. C.; Lohmann, U.; Sierau, B.; Keller, A.; Burtscher, H.; Mensah, A. A.

2015-10-01

Soot particles are the most strongly light-absorbing particles commonly found in the atmosphere. They are major contributors to the radiative budget of the Earth and to the toxicity of atmospheric pollution. Atmospheric aging of soot may change its health- and climate-relevant properties by oxidizing the primary black carbon (BC) or organic particulate matter (OM) which, together with ash, comprise soot. This atmospheric aging, which entails the condensation of secondary particulate matter as well as the oxidation of the primary OM and BC emissions, is currently poorly understood. In this study, atmospheric aging of wood-stove soot aerosols was simulated in a continuous-flow reactor. The composition of fresh and aged soot particles was measured in real time by a dual-vaporizer aerosol-particle mass spectrometer (SP-AMS). The dual-vaporizer SP-AMS provided information on the OM and BC components of the soot as well as on refractory components internally mixed with BC. By switching the SP-AMS laser vaporizer off and using only the AMS thermal vaporizer (at 600 °C), information on the OM component only was obtained. In both modes, OM appeared to be generated largely by cellulose and/or hemicellulose pyrolysis and was only present in large amounts when new wood was added to the stove. In SP-AMS mode, BC signals otherwise dominated the mass spectrum. These signals consisted of ions related to refractory BC (rBC, C1-5+), oxygenated carbonaceous ions (CO1-2+), potassium (K+), and water (H2O+ and related fragments). The C4+ : C3+ ratio, but not the C1+ : C3+ ratio, was consistent with the BC-structure trends of Corbin et al. (2015c). The CO1-2+ signals likely originated from BC surface groups: upon aging, both CO+ and CO2+ increased relative to C1-3+ while CO2+ simultaneously increased relative to CO+. Factor analysis (positive matrix factorization) of SP-AMS and AMS data, using a modified error model to address peak-integration uncertainties, indicated that the surface composition of the BC was approximately constant across all stages of combustion for both fresh and aged samples. These results represent the first time-resolved measurements of in situ BC surface aging and suggest that the surface of beech-wood BC may be modelled as a single chemical species.

Quantitative Surface Emissivity and Temperature Measurements of a Burning Solid Fuel Accompanied by Soot Formation

NASA Technical Reports Server (NTRS)

Piltch, Nancy D.; Pettegrew, Richard D.; Ferkul, Paul; Sacksteder, K. (Technical Monitor)

2001-01-01

Surface radiometry is an established technique for noncontact temperature measurement of solids. We adapt this technique to the study of solid surface combustion where the solid fuel undergoes physical and chemical changes as pyrolysis proceeds, and additionally may produce soot. The physical and chemical changes alter the fuel surface emissivity, and soot contributes to the infrared signature in the same spectral band as the signal of interest. We have developed a measurement that isolates the fuel's surface emissions in the presence of soot, and determine the surface emissivity as a function of temperature. A commercially available infrared camera images the two-dimensional surface of ashless filter paper burning in concurrent flow. The camera is sensitive in the 2 to 5 gm band, but spectrally filtered to reduce the interference from hot gas phase combustion products. Results show a strong functional dependence of emissivity on temperature, attributed to the combined effects of thermal and oxidative processes. Using the measured emissivity, radiance measurements from several burning samples were corrected for the presence of soot and for changes in emissivity, to yield quantitative surface temperature measurements. Ultimately the results will be used to develop a full-field, non-contact temperature measurement that will be used in spacebased combustion investigations.

Soot Formation in Laminar Acetylene/Air Diffusion Flames at Atmospheric Pressure. Appendix C

NASA Technical Reports Server (NTRS)

Xu, F.; Faeth, G. M.; Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2000-01-01

The flame structure and soot-formation (soot nucleation and growth) properties of axisymmetric laminar coflowing jet diffusion flames were studied experimentally. Test conditions involved acetylene-nitrogen jets burning in coflowing air at atmospheric pressure. Measurements were limited to the axes of the flames and included soot concentrations, soot temperatures, soot structure, major gas species concentrations, radical species (H, OH, and O) concentrations, and gas velocities. The results show that as distance increases along the axes of the flames, detectable soot formation begins when significant H concentrations are present, and ends when acetylene concentrations become small. Species potentially associated with soot oxidation-O2, CO2, H2O, O, and OH-are present throughout the soot-formation region so that soot formation and oxidation proceed at the same time. Strong rates of soot growth compared to soot nucleation early in the soot-formation process, combined with increased rates of soot nucleation and oxidation as soot formation proceeds, causes primary soot particle diameters to reach a maximum relatively early in the soot-formation process. Aggregation of primary soot particles proceeds, however, until the final stages of soot oxidation. Present measurements of soot growth (corrected for soot oxidation) in laminar diffusion flames were consistent with earlier measurements of soot growth in laminar premixed flames and exhibited encouraging agreement with existing hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms in the literature that were developed based on measurements within laminar premixed flames. Measured primary soot particle nucleation rates in the present laminar diffusion flames also were consistent with corresponding rates measured in laminar premixed flames and yielded a crude correlation in terms of acetylene and H concentrations and the temperature.

Soot Formation in Laminar Acetylene/Air Diffusion Flames at Atmospheric Pressure. Appendix H

NASA Technical Reports Server (NTRS)

Xu, F.; Faeth, G. M.; Yuan, Z.-G. (Technical Monitor); Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2001-01-01

The flame structure and soot-formation (soot nucleation and growth) properties of axisymmetric laminar coflowing jet diffusion flames were studied experimentally. Test conditions involved acetylene-nitrogen jets burning in coflowing air at atmospheric pressure. Measurements were limited to the axes of the flames and included soot concentrations, soot temperatures, soot structure, major gas species concentrations, radical species (H, OH, and O) concentrations, and gas velocities. The results show that as distance increases along the axes of the flames, detectable soot formation begins when significant H concentrations are present, and ends when acetylene concentrations become small. Species potentially associated with soot oxidation-O2, CO2, H2O, O, and OH-are present throughout the soot-formation region so that soot formation and oxidation proceed at the same time. Strong rates of soot growth compared to soot nucleation early in the soot-formation process, combined with increased rates of soot nucleation and oxidation as soot formation proceeds, causes primary soot particle diameters to reach a maximum relatively early in the soot-formation process. Aggregation of primary soot particles proceeds, however, until the final stages of soot oxidation. Present measurements of soot growth (corrected for soot oxidation) in laminar diffusion flames were consistent with earlier measurements of soot growth in laminar premixed flames and exhibited encouraging agreement with existing hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms in the literature that were developed based on measurements within laminar premixed flames. Measured primary soot particle nucleation rates in the present laminar diffusion flames also were consistent with corresponding rates measured in laminar premixed flames and yielded a crude correlation in terms of acetylene and H concentrations and the temperature.

Soot Formation in Laminar Acetylene/Air Diffusion Flames at Atmospheric Pressure. Appendix J

NASA Technical Reports Server (NTRS)

Xu, F.; Faeth, G. M.; Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2001-01-01

The flame structure and soot-formation (soot nucleation and growth) properties of axisymmetric laminar coflowing jet diffusion flames were studied experimentally. Test conditions involved acetylene-nitrogen jets burning in coflowing air at atmospheric pressure. Measurements were limited to the axes of the flames and included soot concentrations, soot temperatures, soot structure, major gas species concentrations, radical species (H, OH, and O) concentrations, and gas velocities. The results show that as distance increases along the axes of the flames, detectable soot formation begins when significant H concentrations are present, and ends when acetylene concentrations become small. Species potentially associated with soot oxidation--O2, CO2, H2O, O, and OH-are present throughout the soot-formation region so that soot formation and oxidation proceed at the same time. Strong rates of soot growth compared to soot nucleation early in the soot-formation process, combined with increased rates of soot nucleation and oxidation as soot formation proceeds, causes primary soot particle diameters to reach a maximum relatively early in the soot-formation process. Aggregation of primary soot particles proceeds, however, until the final stages of soot oxidation. Present measurements of soot growth (corrected for soot oxidation) in laminar diffusion flames were consistent with earlier measurements of soot growth in laminar premixed flames and exhibited encouraging agreement with existing hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms in the literature that were developed based on measurements within laminar premixed flames. Measured primary soot particle nucleation rates in the present laminar diffusion flames also were consistent with corresponding rates measured in laminar premixed flames and yielded a crude correlation in terms of acetylene and H concentrations and the temperature.

An Atmospheric Atomic Oxygen Source for Cleaning Smoke Damaged Art Objects

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Rutledge, Sharon K.; Norris, Mary Jo

1998-01-01

Soot and other carbonaceous combustion products deposited on the surfaces of porous ceramic, stone, ivory and paper can be difficult to remove and can have potentially unsatisfactory results using wet chemical and/or abrasive cleaning techniques. An atomic oxygen source which operates in air at atmospheric pressure, using a mixture of oxygen and helium, has been developed to produce an atomic oxygen beam which is highly effective in oxidizing soot deposited on surfaces by burning candles made of paraffin, oil or rendered animal fat. Atomic oxygen source operating conditions and the results of cleaning soot from paper, gesso, ivory, limestone and water color-painted limestone are presented,

First in-flight synchrotron X-ray absorption and photoemission study of carbon soot nanoparticles

PubMed Central

Ouf, F.-X.; Parent, P.; Laffon, C.; Marhaba, I.; Ferry, D.; Marcillaud, B.; Antonsson, E.; Benkoula, S.; Liu, X.-J.; Nicolas, C.; Robert, E.; Patanen, M.; Barreda, F.-A.; Sublemontier, O.; Coppalle, A.; Yon, J.; Miserque, F.; Mostefaoui, T.; Regier, T. Z.; Mitchell, J.-B. A.; Miron, C.

2016-01-01

Many studies have been conducted on the environmental impacts of combustion generated aerosols. Due to their complex composition and morphology, their chemical reactivity is not well understood and new developments of analysis methods are needed. We report the first demonstration of in-flight X-ray based characterizations of freshly emitted soot particles, which is of paramount importance for understanding the role of one of the main anthropogenic particulate contributors to global climate change. Soot particles, produced by a burner for several air-to-fuel ratios, were injected through an aerodynamic lens, focusing them to a region where they interacted with synchrotron radiation. X-ray photoelectron spectroscopy and carbon K-edge near-edge X-ray absorption spectroscopy were performed and compared to those obtained for supported samples. A good agreement is found between these samples, although slight oxidation is observed for supported samples. Our experiments demonstrate that NEXAFS characterization of supported samples provides relevant information on soot composition, with limited effects of contamination or ageing under ambient storage conditions. The highly surface sensitive XPS experiments of airborne soot indicate that the oxidation is different at the surface as compared to the bulk probed by NEXAFS. We also report changes in soot’s work function obtained at different combustion conditions. PMID:27883014

Numerical modelling of soot formation and oxidation in laminar coflow non-smoking and smoking ethylene diffusion flames

NASA Astrophysics Data System (ADS)

Liu, Fengshan; Guo, Hongsheng; Smallwood, Gregory J.; Gülder, Ömer L.

2003-06-01

A numerical study of soot formation and oxidation in axisymmetric laminar coflow non-smoking and smoking ethylene diffusion flames was conducted using detailed gas-phase chemistry and complex thermal and transport properties. A modified two-equation soot model was employed to describe soot nucleation, growth and oxidation. Interaction between the gas-phase chemistry and soot chemistry was taken into account. Radiation heat transfer by both soot and radiating gases was calculated using the discrete-ordinates method coupled with a statistical narrow-band correlated-k based band model, and was used to evaluate the simple optically thin approximation. The governing equations in fully elliptic form were solved. The current models in the literature describing soot oxidation by O2 and OH have to be modified in order to predict the smoking flame. The modified soot oxidation model has only moderate effects on the calculation of the non-smoking flame, but dramatically affects the soot oxidation near the flame tip in the smoking flame. Numerical results of temperature, soot volume fraction and primary soot particle size and number density were compared with experimental data in the literature. Relatively good agreement was found between the prediction and the experimental data. The optically thin approximation radiation model significantly underpredicts temperatures in the upper portion of both flames, seriously affecting the soot prediction.

Water interaction with laboratory-simulated fossil fuel combustion particles.

PubMed

Popovicheva, O B; Kireeva, E D; Shonija, N K; Khokhlova, T D

2009-10-01

To clarify the impact of fossil fuel combustion particles' composition on their capacity to take up water, we apply a laboratory approach in which the method of deposition of compounds, identified in the particulate coverage of diesel and aircraft engine soot particles, is developed. It is found that near-monolayer organic/inorganic coverage of the soot particles may be represented by three groups of fossil fuel combustion-derived particulate matter with respect to their Hansh's coefficients related to hydrophilic properties. Water adsorption measurements show that nonpolar organics (aliphatic and aromatic hydrocarbons) lead to hydrophobization of the soot surface. Acidic properties of organic compounds such as those of oxidized PAHs, ethers, ketones, aromatic, and aliphatic acids are related to higher water uptake, whereas inorganic acids and ionic compounds such as salts of organic acids are shown to be responsible for soot hydrophilization. This finding allows us to quantify the role of the chemical identity of soot surface compounds in water uptake and the water interaction with fossil fuel combustion particles in the humid atmosphere.

Atomic Oxygen Treatment as a Method of Recovering Smoke Damaged Paintings. Revised

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Banks, Bruce A.; Forkapa, Mark; Stueber, Thomas; Sechkar, Edward; Malinowski, Kevin

1999-01-01

A noncontact technique is described that uses atomic oxygen, generated under low pressure in the presence of nitrogen, to remove soot and charred varnish from the surface of a painting. The process, which involves surface oxidation, permits control of the amount of surface material removed. The effectiveness of the process was evaluated by reflectance measurements from selected areas made during the removal of soot from acrylic gesso, ink on paper, and varnished oil paint substrates. For the latter substrate, treatment also involved the removal of damaged varnish and paint binder from the surface.

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

NASA Astrophysics Data System (ADS)

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 adsorptive and reactive centers on soot surface where NO2 is converted into HONO and other products. Coating the soot surface by different materials to simulate atmospheric aging has a strong impact on the reactivity of soot toward NO2. Sulfuric acid coating reduces the uptake coefficient and HONO production by physically blocking the soot active sites and initiating decomposition of HONO in the aqueous acid layer. Furthermore, the HONO yield can be reduced to zero after exposure to elevated relative humidity or partially restored when sulfuric acid is removed by heating. Coatings made of glutaric and succinic acids increase HONO yields and NO2 uptake coefficients, similarly as in the case of pre-heated soot samples. We propose that the organic acids change the top layer morphology, opening up the pores and making the internal soot surface more accessible for heterogeneous interaction with NO2. The implications of our study regarding the contribution of freshly emitted and aged soot aerosols to nighttime HONO production will be discussed.

Understanding the difference in oxidative properties between flame and diesel soot nanoparticles: the role of metals.

PubMed

Kim, S H; Fletcher, R A; Zachariah, M R

2005-06-01

The purpose of this paper is to address the differences observed in the oxidative kinetics between flame and diesel derived soots. In particular, it has been observed that flame soot has a significantly higher activation energy for oxidation than does diesel soot. The hypothesis tested in this paper is that metals, possibly coming from lubricating oils, within diesel generated soot particles may be responsible for this effect. This is supported by the fact that addition of metal additives to diesel fuel is shown to have no effect on the activation energy of soot oxidation. The subject of this paper lies in testing the hypothesis by adding metal directly to a flame and extracting oxidation kinetics. Using a high temperature oxidation tandem differential mobility analyzer (HTO-TDMA) we extract particle size dependent kinetics for the oxidation of flame-derived soot doped with and without iron. We found that indeed addition of iron to a flame reduced the activation energy significantly from approximately 162 +/- 3 kJ/mol to approximately 116 +/- 3 kJ/mol, comparable with diesel engine generated soot with an activation energy approximately 110 kJ/mol. These results are consistent with the idea that small quantities of metals during diesel combustion may play an important role in soot abatement.

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

NASA Astrophysics Data System (ADS)

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 important factor governing the soot reactivity. In the third phase of this research, diesel soot was generated under 0 and 20% EGR using a four-cylinder, four-stroke, turbocharged common rail direct injection (DI) DDC diesel engine. The objective of this work was to examine the relevance of the single cylinder engine and flame studies to practical engine operation. The key engine parameters such as load, speed, and injection timing were kept constant to isolate the EGR effect on soot properties from any other engine effects. The thermokinetic analyses of the flame soot and engine soot showed a significant increase in soot oxidation rate as a result of the CO2 or EGR inclusion into the combustion process. The activation energy of soot oxidation was found to be independent of soot origin or formation history. The increase in soot oxidation rate is attributed solely to the increase in soot active sites, which are presented implicitly in the pre-exponential factor (A) of the oxidation rate equation. This latter statement was confirmed by measuring the initial active site area (ASA i) of all soot samples considered in this study. As expected, higher oxidation rates are associated with higher ASAi. The chemical properties of the soot were investigated to determine their effects upon soot reactivity. The results showed that the H/C and O/C ratios were not modified by CO2 or EGR addition. Therefore, these ratios are not reactivity parameters and their effects upon soot reactivity were ruled out. In distinct contrast, the physical properties of the soot were modified by the addition of CO2 or EGR. The interlayer spacing (d002) between the aromatic sheets increased, the crystallite width (La) decreased and the crystallite height (Lc) decreased as a consequence of CO 2 or EGR addition. The modified physical properties of the soot are responsible for the increased rate of soot oxidation. In order to examine the soot oxidation behavior in the DPF, the soot samples produced from the DDC engine under 0 and 20% EGR were partially oxidized in a thermogravimetric analyzer (TGA) to specific conversion levels. Unreacted and partially oxidized soot samples were then subjected to comprehensive characterization. The Raman spectroscopy showed that the disordered fraction of the soot (ID/IG) decreases with the oxidation progression. Electron energy loss spectroscopy (EELS) results showed an increase in the (I pi/Isigma) for soot generated under 0% EGR but no significant increase in this ratio was observed for the soot generated under 20% EGR. These results indicate that soot generated without EGR is likely to be more highly ordered in its nanostructure. Visual inspection of the unreacted and partially oxidized soot (produced under 0 and 20% EGR) was obtained by the use of high resolution transmission electron microscopy (HRTEM). The results suggested that the initial nanostructure of the soot primary particles is the same for soot produced under 0 and 20% EGR. However, soot produced under 0% EGR condition exhibits strictly external burning (i.e., from the outside in). On the other hand, soot generated under 20% EGR possesses dual burning modes, that is, slow external burning and fast internal burning. This internal burning of the 20% EGR soot clarifies the importance of the burning modes upon soot reactivity. This study confirmed that EGR exerted a strong influence on the diesel soot physical properties. Consistent with the flame study, a separate engine study confirmed that the most important factors to enhance the soot reactivity are the thermal effect of the EGR followed by the dilution effect.

Effects of Soot Structure on Soot Oxidation Kinetics

DTIC Science & Technology

2011-06-01

information from PSDs, temperature, gas -phase composition was used to develop an oxidation kinetic expression that accounts for the effects of...from PSDs, temperature, gas -phase composition was used to develop an oxidation kinetic expression that accounts for the effects of temperature, O2, and...systematic studies of these effects under the temperatures and times of interest to soot oxidation in gas turbine engines. Studies have shown that soot

Effects of Gravity on Soot Formation in a Coflow Laminar Methane/Air Diffusion Flame

NASA Astrophysics Data System (ADS)

Kong, Wenjun; Liu, Fengshan

2010-04-01

Simulations of a laminar coflow methane/air diffusion flame at atmospheric pressure are conducted to gain better understanding of the effects of gravity on soot formation by using detailed gas-phase chemistry, complex thermal and transport properties coupled with a semiempirical two-equation soot model and a nongray radiation model. Soot oxidation by O2, OH and O was considered. Thermal radiation was calculated using the discrete ordinate method coupled with a statistical narrow-band correlated-K model. The spectral absorption coefficient of soot was obtained by Rayleigh's theory for small particles. The results show that the peak temperature decreases with the decrease of the gravity level. The peak soot volume fraction in microgravity is about twice of that in normal gravity under the present conditions. The numerical results agree very well with available experimental results. The predicted results also show that gravity affects the location and intensity for soot nucleation and surface growth.

Soot Combustion over Nanostructured Ceria with Different Morphologies

PubMed Central

Zhang, Wen; Niu, Xiaoyu; Chen, Liqiang; Yuan, Fulong; Zhu, Yujun

2016-01-01

In this study, nano-structure ceria with three different morphologies (nanorod, nanoparticle and flake) have been prepared by hydrothermal and solvothermal methods. The ceria samples were deeply characterized by XRD, SEM, TEM, H2-TPR, XPS and in-situ DRIFTS, and tested for soot combustion in absence/presence NO atmospheres under loose and tight contact conditions. The prepared ceria samples exhibit excellent catalytic activities, especially, the CeO2 with nanorod (Ce-R) shows the best catalytic activity, for which the peak temperature of soot combustion (Tm) is about 500 and 368 °C in loose and tight contact conditions, respectively. The catalytic activity for Ce-R is higher than that of the reported CeO2 catalysts and reaches a level that of precious metals. The characterization results reveal that the maximal amounts of adsorbed oxygen species on the surface of the nanostructure Ce-R catalyst should be the crucial role to decide the catalytic soot performance. High BET surface area may also be a positive effect on soot oxidation activity under loose contact conditions. PMID:27353143

[Catalytic combustion of soot on combined oxide catalysts].

PubMed

He, Xu-wen; Yu, Jun-jie; Kang, Shou-fang; Hao, Zheng-ping; Hu, Chun

2005-01-01

Combined oxide catalysts are prepared for catalytic combustion of soot and regeneration from diesel emissions. Thermo-gravimetric analysis(TGA) and temperature programmed oxidation(TPO)are used to evaluate the activity of catalysts under the influence of composition,atomic ration, H2O, calcinations temperature and mass ration between catalysts and soot. Results show that Cu-Mo-O had high activity among double metal oxide catalysts. Among multicomponent metal oxide catalysts, Cu-K-Mo-O had high activity when atomic ratio Cu: K: Mo = 1:1:2 and mass ration between catalysts and soot equals 5: 1. Under this condition, soot ignition temperature of Cu-K-Mo-O catalyst was 327 degrees C. H2O addition and calcinations temperature had little influence on it,which is one kind of compatible catalyst for soot control and catalytic regeneration from diesel emissions.

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

PubMed

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 temperatures

Cleaning of Fire Damaged Watercolor and Textiles Using Atomic Oxygen

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Banks, Bruce A.; Chichernea, Virgil A.; Haytas, Christy A.

2000-01-01

A noncontact technique is described that uses atomic oxygen generated under low pressure in the presence of nitrogen to remove soot from the surface of a test watercolor panel and strips of cotton, wool and silk. The process, which involves surface oxidation, permits control of the amount of surface material removed. The effectiveness of soot removal from test panels of six basic watercolors (alizarin crimson, burnt sienna, lemon yellow, yellow ochre, cerulean blue and ultramarine blue) and strips of colored cotton, wool and silk was measured using reflectance spectroscopy. The atomic oxygen removed soot effectively from the treated areas and enabled partial recovery of charred watercolors. However, overexposure can result in removal of sizing, bleaching, and weakening of the structure. With the proper precautions, atomic oxygen treatment appears to have great potential to salvage heavily smoke damaged artworks which were previously considered unrestorable.

Key role of organic carbon in the sunlight-enhanced atmospheric aging of soot by O2

PubMed Central

Han, Chong; Liu, Yongchun; Ma, Jinzhu; He, Hong

2012-01-01

Soot particles are ubiquitous in the atmosphere and have important climatic and health effects. The aging processes of soot during long-range transport result in variability in its morphology, microstructure, and hygroscopic and optical properties, subsequently leading to the modification of soot’s climatic and health effects. In the present study the aging process of soot by molecular O2 under simulated sunlight irradiation is investigated. Organic carbon components on the surface of soot are found to play a key role in soot aging and are transformed into oxygen-containing organic species including quinones, ketones, aldehydes, lactones, and anhydrides. These oxygen-containing species may become adsorption centers of water and thus enhance the cloud condensation nuclei and ice nuclei activities of soot. Under irradiation of 25 mW·cm−2, the apparent rate constants (k1,obs) for loss or formation of species on soot aged by 20% O2 were larger by factors of 1.5–3.5 than those on soot aged by 100 ppb O3. Considering the abundance of O2 in the troposphere and its higher photoreactivity rate, the photochemical oxidation by O2 under sunlight irradiation should be a very important aging process for soot. PMID:23236134

Evaluation and optimisation of phenomenological multi-step soot model for spray combustion under diesel engine-like operating conditions

NASA Astrophysics Data System (ADS)

Pang, Kar Mun; Jangi, Mehdi; Bai, Xue-Song; Schramm, Jesper

2015-05-01

In this work, a two-dimensional computational fluid dynamics study is reported of an n-heptane combustion event and the associated soot formation process in a constant volume combustion chamber. The key interest here is to evaluate the sensitivity of the chemical kinetics and submodels of a semi-empirical soot model in predicting the associated events. Numerical computation is performed using an open-source code and a chemistry coordinate mapping approach is used to expedite the calculation. A library consisting of various phenomenological multi-step soot models is constructed and integrated with the spray combustion solver. Prior to the soot modelling, combustion simulations are carried out. Numerical results show that the ignition delay times and lift-off lengths exhibit good agreement with the experimental measurements across a wide range of operating conditions, apart from those in the cases with ambient temperature lower than 850 K. The variation of the soot precursor production with respect to the change of ambient oxygen levels qualitatively agrees with that of the conceptual models when the skeletal n-heptane mechanism is integrated with a reduced pyrene chemistry. Subsequently, a comprehensive sensitivity analysis is carried out to appraise the existing soot formation and oxidation submodels. It is revealed that the soot formation is captured when the surface growth rate is calculated using a square root function of the soot specific surface area and when a pressure-dependent model constant is considered. An optimised soot model is then proposed based on the knowledge gained through this exercise. With the implementation of optimised model, the simulated soot onset and transport phenomena before reaching quasi-steady state agree reasonably well with the experimental observation. Also, variation of spatial soot distribution and soot mass produced at oxygen molar fractions ranging from 10.0 to 21.0% for both low and high density conditions are reproduced.

Determination of kinetic data for soot oxidation: Modeling of competition between oxygen diffusion and reaction during thermogravimetric analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gilot, P.; Bonnefoy, F.; Marcuccilli, F.

1993-10-01

Kinetic data concerning carbon black oxidation in the temperature range between 600 and 900 C have been obtained using thermogravimetric analysis. Modeling of diffusion in a boundary layer above the pan and inside the porous medium coupled to oxygen reaction with carbon black is necessary to obtain kinetic constants as a function of temperature. These calculations require the knowledge of the oxidation rate at a given constant temperature as a function of the initial mass loading m[sub o]. This oxidation rate, expressed in milligrams of soot consumed per second and per milligram of initial soot loading, decreases when m[sub o]more » increases, in agreement with a reaction in an intermediary regime where the kinetics and the oxygen diffusion operate. The equivalent diffusivity of oxygen inside the porous medium is evaluated assuming two degrees of porosity: between soot aggregates and inside each aggregate. Below 700 C an activation energy of about 103 kJ/mol can be related to a combustion reaction probably kinetically controlled. Beyond 700 C the activation energy of about 20 kJ/ mol corresponds to a reaction essentially controlled by oxygen diffusion leading to a constant density oxidation with oxygen consumption at or near the particle surface. To validate these data, they are used in the modeling of a Diesel particulate trap regeneration. In this particular case, the oxidizing flux is forced across the carbon black deposit, oxygen diffusion being insignificant. A good agreement between experimental results and model predictions is obtained, proving the rate constants validity.« less

Diamonds in detonation soot

NASA Technical Reports Server (NTRS)

Greiner, N. Roy; Phillips, Dave; Johnson, J. D.; Volk, Fred

1990-01-01

Diamonds 4 to 7 nm in diameter have been identified and partially isolated from soot formed in detonations of carbon-forming composite explosives. The morphology of the soot has been examined by transmission electron microscopy (TEM), and the identity of the diamond has been established by the electron diffraction pattern of the TEM samples and by the X-ray diffraction (XRD) pattern of the isolated solid. Graphite is also present in the form of ribbons of turbostatic structure with a thickness of 2 to 4 nm. A fraction, about 25 percent of the soot by weight, was recovered from the crude soot after oxidation of the graphite with fuming perchloric acid. This fraction showed a distinct XRD pattern of diamond and the diffuse band of amorphous carbon. The IR spectrum of these diamonds closely matches that of diamonds recovered from meteorites (Lewis et al., 1987), perhaps indicating similar surface properties after the oxidation. If these diamonds are produced in the detonation itself or during the initial expansion, they exhibit a phenomenal crystal growth rate (5 nm/0.00001 s equal 1.8 m/hr) in a medium with a very low hydrogen/carbon ratio. Because the diamonds will be carried along with the expanding gases, they will be accelerated to velocities approaching 8 km/s.

Method for removing soot from exhaust gases

DOE Office of Scientific and Technical Information (OSTI.GOV)

Suib, Steven L.; Dharmarathna, D. A. Saminda; Pahalagedara, Lakshitha R.

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 andmore » 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).« less

Shock tube study of the fuel structure effects on the chemical kinetic mechanisms responsible for soot formation

NASA Technical Reports Server (NTRS)

Frenklach, M.

1983-01-01

Soot formation in toluene-, benzene-, and acetylene-oxygen-argon mixtures was investigated to study soot formation in a combustion environment. High concentrations of oxygen completely suppress soot formation. The addition of oxygen at relatively low concentrations uniformly suppresses soot formation at high pressures, while at relatively lower pressures it suppresses soot formation at higher temperatures while promoting soot production at lower temperatures. The observed behavior indicates that oxidation reactions compete with ring fragmentation. The main conclusion to be drawn from the results is that the soot formation mechanism is probably the same for the pyrolysis and oxidation of hydrocarbons. That is, the addition of oxygen does not alter the soot route but rather promotes or inhibits this route by means of competitive reactions. An approach to empirical modeling of soot formation during pyrolysis of aromatic hydrocarbons is also presented.

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

PubMed

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.

Modelling of soot formation in laminar diffusion flames using a comprehensive CFD-PBE model with detailed gas-phase chemistry

NASA Astrophysics Data System (ADS)

Akridis, Petros; Rigopoulos, Stelios

2017-01-01

A discretised population balance equation (PBE) is coupled with an in-house computational fluid dynamics (CFD) code in order to model soot formation in laminar diffusion flames. The unsteady Navier-Stokes, species and enthalpy transport equations and the spatially-distributed discretised PBE for the soot particles are solved in a coupled manner, together with comprehensive gas-phase chemistry and an optically thin radiation model, thus yielding the complete particle size distribution of the soot particles. Nucleation, surface growth and oxidation are incorporated into the PBE using an acetylene-based soot model. The potential of the proposed methodology is investigated by comparing with experimental results from the Santoro jet burner [Santoro, Semerjian and Dobbins, Soot particle measurements in diffusion flames, Combustion and Flame, Vol. 51 (1983), pp. 203-218; Santoro, Yeh, Horvath and Semerjian, The transport and growth of soot particles in laminar diffusion flames, Combustion Science and Technology, Vol. 53 (1987), pp. 89-115] for three laminar axisymmetric non-premixed ethylene flames: a non-smoking, an incipient smoking and a smoking flame. Overall, good agreement is observed between the numerical and the experimental results.

The Role of Biogenic and Anthropogenic Hydrocarbons in Aging of Atmospheric Soot

NASA Astrophysics Data System (ADS)

Khalizov, A. F.; Qiu, C.; Lin, Y.; Ma, Y.; Wang, L.; Zhang, R.

2012-12-01

Atmospheric soot is often found to be internally mixed with other aerosol constituents, yet the processes responsible for the soot aging are not well understood. We have conducted a systematic study on the role of several representative biogenic and anthropogenic volatile organic compounds (VOCs), including monoterpenes and aromatics, in atmospheric aging of combustion soot. Aging experiments were conducted in a fluoropolymer chamber on size-classified soot aerosols in the presence of a VOC and an oxidant, either ozone or photolytically generated hydroxyl radical (OH). The evolution in the aging state of soot was monitored from measurements of the particle mobility size and mass, which were used to derive information about particle effective density, dynamic shape factor, and coating thickness. When exposed to VOC and oxidant, soot particles promptly gain mass due to condensation of low-volatility and partitioning of semi-volatile VOC oxidation products. Depending on the VOC, the increase in the particle mass is accompanied by an increase or a decrease in the particle mobility diameter. In either case, the effective density of coated soot particles increases during aging because the condensed material fills in the voids of fractal soot aggregates, forcing their restructuring. The latter is confirmed by thermal denuding experiments, which show an increase in the effective density for soot that was first aged and then heated to remove the coating from the soot core. Hygroscopic and optical properties of soot are significantly altered by aging. Upon humidification, the coating absorbs water, increasing in volume and causing an additional restructuring of soot aggregates. Coated particles are sufficiently hygroscopic to activate to cloud droplets at atmospherically relevant water supersaturations. Aged soot shows stronger light absorption and scattering, with an enhancement magnitude depending on the coating thickness and nature of the coating precursor. The rate of aging and corresponding changes in the properties of soot are enhanced in the presence of nitrogen oxides (NOx = NO + NO2), a common combustion co-pollutant of soot. On the basis of our experimental results we conclude that biogenic and anthropogenic VOCs play a significant role in the atmospheric aging of combustion soot, shortening its atmospheric lifetime while enhancing impacts on air quality and climate.

Morphological study of fluorescent carbon Nanoparticles (F-CNPs) from ground coffee waste soot oxidation by diluted acid

NASA Astrophysics Data System (ADS)

Gea, S.; Tjandra, S.; Joshua, J.; Wirjosentono, B.

2018-02-01

Coffee ground waste utilization for fluorescent carbon nanoparticles (F-CNPs) through soot oxidation with diluted HNO3 has been conducted. Soot was obtained through three different treatments to coffee ground waste; which was burned in furnaceat 550°C and 650°C and directly burned in a heat-proofcontainer. Then they were analyzed morphologically with Scanning Electron Microscope (SEM) instrument. Soot from direct burning indicated the optimum result where it has denser pores compared to other two soots. Soot obtained from direct burning was refluxed in diluted HNO3 for 12 hours to perform the oxidation. Yellowish brown supernatant was later observed which lead to green fluorescent under the UV light. F-CNPs characterization was done in Transmission Electron Microscopy, which showed that 7.4-23.4 nm of particle size were distributed.

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

NASA Astrophysics Data System (ADS)

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 morphology, which was further confirmed from the STEM image. Moreover, it was found that volume equivalent coating thickness (Δrve) could also be applied to normalized characterize soot aging parameters like diameter growth factor (Gfd) and mass growth factor (Gfm) in a complex reaction system like isoprene/SO2/NOx. Our results revealed the dual mechanism (competitive effect&cooperative effect) of isoprene and SO2 on photochemical aging of soot, which is of significance for improving understanding of complex air pollution in China.

Particulate morphology of waste cooking oil biodiesel and diesel in a heavy duty diesel engine

NASA Astrophysics Data System (ADS)

Hwang, Joonsik; Jung, Yongjin; Bae, Choongsik

2014-08-01

The effect of biodiesel produced from waste cooking oil (WCO) on the particulate matters (PM) of a direct injection (DI) diesel engine was experimentally investigated and compared with commercial diesel fuel. Soot agglomerates were collected with a thermophoretic sampling device installed in the exhaust pipe of the engine. The morphology of soot particles was analyzed using high resolution transmission electron microscopy (TEM). The elemental and thermogravimetric analysis (TGA) were also conducted to study chemical composition of soot particles. Based on the TEM images, it was revealed that the soot derived from WCO biodiesel has a highly graphitic shell-core arrangement compared to diesel soot. The mean size was measured from averaging 400 primary particles for WCO biodiesel and diesel respectively. The values for WCO biodiesel indicated 19.9 nm which was smaller than diesel's 23.7 nm. From the TGA results, WCO biodiesel showed faster oxidation process. While the oxidation of soot particles from diesel continued until 660°C, WCO biodiesel soot oxidation terminated at 560°C. Elemental analysis results showed that the diesel soot was mainly composed of carbon and hydrogen. On the other hand, WCO biodiesel soot contained high amount of oxygen species.

Oxidation of diesel soot on binary oxide CuCr(Co)-based monoliths.

PubMed

Soloviev, Sergiy O; Kapran, Andriy Y; Kurylets, Yaroslava P

2015-02-01

Binary oxide systems (CuCr2O4, CuCo2O4), deposited onto cordierite monoliths of honeycomb structure with a second support (finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot using internal combustion engine's gas exhausts (O2, NOx, H2O, CO2) and O3 as oxidizing agents. It is shown that the second support increases soot capacity of aforementioned filters, and causes dispersion of the particles of spinel phases as active components enhancing thereby catalyst activity and selectivity of soot combustion to CO2. Oxidants used can be arranged with reference to decreasing their activity in a following series: O3≫NO2>H2O>NO>O2>CO2. Ozone proved to be the most efficient oxidizing agent: the diesel soot combustion by O3 occurs intensively (in the presence of copper chromite based catalyst) even at closing to ambient temperatures. Results obtained give a basis for the conclusion that using a catalytic coating on soot filters in the form of aforementioned binary oxide systems and ozone as the initiator of the oxidation processes is a promising approach in solving the problem of comprehensive purification of automotive exhaust gases at relatively low temperatures, known as the "cold start" problem. Copyright © 2014. Published by Elsevier B.V.

Effects of Structure and Hydrodynamics on the Sooting Behavior of Spherical Microgravity Diffusion Flames

NASA Technical Reports Server (NTRS)

Sunderland, P. B.; Axelbaum, R. L.; Urban, D. L.

1999-01-01

Recent experimental, numerical and analytical work has shown that the stoichiometric mixture fraction (Z(sub st)) can have a profound effect on soot formation in diffusion flames. These findings were obtained at constant flame temperature (T(sub ad)), employing the approach described in Du and Axelbaum (1995, 1996). For example, a fuel mixture containing 1 mole of ethylene and 11.28 moles of nitrogen burning in pure oxygen ((Z(sub st)) = 0.78) has the same adiabatic flame temperature (2370 K) as that of pure ethylene burning in air ((Z(sub st)) = 0.064). An important finding of these works was that at sufficiently high (Z(sub st)), flames remain blue as strain rate approaches zero in counterflow flames, or as flame height and residence time approach infinity in coflowing flames. Lin and Faeth (1996a) coined the term permanently blue to describe such flames. Two theories have been proposed to explain the appearance of permanently-blue flames at high (Z(sub st)). They are based on (1) hydrodynamics and (2) flame structure. Previous experimental studies in normal gravity are not definitive as to which, if either, mechanism is dominant because both hydrodynamics and structure suppress soot formation at high (Z(sub st)) in coflowing and counterflowing diffusion flames. In counterflow flames with (Z(sub st)) < 0.5 streamlines at the flame sheet are directed toward the fuel. Newly formed soot is convected into richer regions, favoring soot growth over oxidation. For (Z(sub st)) > 0.5, convection at the flame is toward the oxidizer, thus enhancing soot oxidization. Thus, in counterflow flames, hydrodynamics causes soot to be convected towards the oxidizer at high (Z(sub st)) which suppresses soot formation. Axelbaum and co-workers maintain that while the direction of convection can impact soot growth and oxidation, these processes alone cannot cause permanently-blue flames. Soot growth and oxidation are dependent on the existence of soot particles and the presence of soot is invariably accompanied by yellow luminosity. Soot-particle inception, on the other hand, arises from gas-phase reactions and its dependence on flow direction is weak, similar to that of other gas-phase reactions in flames. For example, when the flame moves across the stagnation plane no significant changes in flame chemistry are observed. Furthermore, since the soot-inception zone has a finite thickness, soot has been produced in counterflow flames with (Z(sub st)) > 0.5. For large (Z(sub st)) the fuel concentration decreases and oxygen concentration increases in the soot forming regions of the flame. This yields a shift in the OH profile toward the fuel side of the flame, and this shift can dramatically influence soot inception because it essentially narrows the soot inception zone. Soot-free (permanently-blue) conditions can be realized when the structure of the flame is adjusted to the extent that significant oxidizing species exist on the fuel side of the flame at temperatures above the critical temperature for soot inception, ca. 1250 K. In previously considered flames it was impossible to independently vary flame structure and convection direction. In contrast, spherical diffusion flames (which generally require microgravity) allow both properties to be varied independently. We altered structure (Z(sub st)) by exchanging inert between the oxidizer and the fuel and we independently varied convection direction at the flame sheet by interchanging the injected and ambient gases. In this work we established four flames: (a) ethylene issuing into air, (b) diluted ethylene issuing into oxygen, (c) air issuing into ethylene, and (d) oxygen issuing into diluted ethylene. (Z(sub st)) is 0.064 in flames (a) and (c) and 0.78 in flames (b) and (d). The convection direction is from fuel to oxidizer in flames (a) and (b) and from oxidizer to fuel in flames (c) and (d). Under the assumption of equal diffusivities of all species and heat, the stoichiometric contours of these flames have identical temperatures and nitrogen concentrations.

The effect of soot modeling on thermal radiation in buoyant turbulent diffusion flames

NASA Astrophysics Data System (ADS)

Snegirev, A.; Kokovina, E.; Tsoy, A.; Harris, J.; Wu, T.

2016-09-01

Radiative impact of buoyant turbulent diffusion flames is the driving force in fire development. Radiation emission and re-absorption is controlled by gaseous combustion products, mainly CO2 and H2O, and by soot. Relative contribution of gas and soot radiation depends on the fuel sooting propensity and on soot distribution in the flame. Soot modeling approaches incorporated in big commercial codes were developed and calibrated for momentum-dominated jet flames, and these approaches must be re-evaluated when applied to the buoyant flames occurring in fires. The purpose of this work is to evaluate the effect of the soot models available in ANSYS FLUENT on the predictions of the radiative fluxes produced by the buoyant turbulent diffusion flames with considerably different soot yields. By means of large eddy simulations, we assess capability of the Moss-Brooks soot formation model combined with two soot oxidation submodels to predict methane- and heptane-fuelled fires, for which radiative flux measurements are available in the literature. We demonstrate that the soot oxidation models could be equally important as soot formation ones to predict the soot yield in the overfire region. Contribution of soot in the radiation emission by the flame is also examined, and predicted radiative fluxes are compared to published experimental data.

Chemical mechanisms of photocatalytic de-soiling and de-polluting processes in indoor environments and urban surfaces

NASA Astrophysics Data System (ADS)

Sleiman, M.; Rosseler, O.; Montesinos, N.; Litter, M.; Bikiel, D.; Kirchstetter, T.; Bluhm, H.; Ahmed, M.; Salmeron, M.; Destaillats, H.

2013-12-01

Photocatalysis has been postulated as a promising approach for the de-pollution of indoor air and urban atmospheres, and for self-cleaning surfaces. Building materials and coatings containing nano-sized TiO2 photocatalytic functionalities are gaining market share, including self-cleaning building envelope materials (coatings, mortar, plaster, architectural fabrics and tiles) and indoor air purifiers. While many studies have reported good performance of photocatalysis in the removal of organic pollutants from indoor air, more information is needed to understand secondary emissions of potentially harmful byproducts from photocatalytic air cleaners. This presentation will describe analytical methods and experimental results from room-sized chamber experiments using a realistic challenge VOC mixture at low ppb levels. We will also present results from separate studies that used synchrotron-based surface spectroscopic and mass spectrometric methods to better understand the photocatalytic mechanisms that regulate the de-soiling and de-polluting activity. Two photocatalytic processes were studied: de-noxification (NOx removal) and de-soiling (removal of deposited black carbon or soot). Ambient pressure XPS was used to study surface and gas-phase species formed during adsorption of NO2 on TiO2 and subsequent UV irradiation at λ = 365 nm. The results illustrate how NOx chemistry on TiO2 surfaces can be affected by the presence of water vapor, heteroatoms present as impurities, and carbonaceous soiling. The reactivity of NOx and NO3- on surfaces leads to reduced adsorbed and gas-phase nitrogenated species. These processes need to be considered in the engineering of depolluting materials and incorporated into atmospheric models. De-soiling properties were investigated by analyzing soot oxidation on TiO2 surfaces. Model soot samples were used as surrogates of urban grime. Using laser desorption coupled with time-of-flight (TOF) mass spectrometry synchrotron ionization, we investigated the mechanisms of photocatalytic soot removal under UVA irradiation. Ancillary reflectance measurements were performed to determine the efficiency and kinetics of soot removal.

Analysis of turbulence and surface growth models on the estimation of soot level in ethylene non-premixed flames

NASA Astrophysics Data System (ADS)

Yunardi, Y.; Munawar, Edi; Rinaldi, Wahyu; Razali, Asbar; Iskandar, Elwina; Fairweather, M.

2018-02-01

Soot prediction in a combustion system has become a subject of attention, as many factors influence its accuracy. An accurate temperature prediction will likely yield better soot predictions, since the inception, growth and destruction of the soot are affected by the temperature. This paper reported the study on the influences of turbulence closure and surface growth models on the prediction of soot levels in turbulent flames. The results demonstrated that a substantial distinction was observed in terms of temperature predictions derived using the k-ɛ and the Reynolds stress models, for the two ethylene flames studied here amongst the four types of surface growth rate model investigated, the assumption of the soot surface growth rate proportional to the particle number density, but independent on the surface area of soot particles, f ( A s ) = ρ N s , yields in closest agreement with the radial data. Without any adjustment to the constants in the surface growth term, other approaches where the surface growth directly proportional to the surface area and square root of surface area, f ( A s ) = A s and f ( A s ) = √ A s , result in an under- prediction of soot volume fraction. These results suggest that predictions of soot volume fraction are sensitive to the modelling of surface growth.

On Soot Inception in Nonpremixed Flames and the Effects of Flame Structure

NASA Technical Reports Server (NTRS)

Chao, B. H.; Liu, S.; Axelbaum, R. L.; Gokoglu, Suleyman (Technical Monitor)

1998-01-01

A simplified three-step model of soot inception has been employed with high activation energy asymptotics to study soot inception in nonpremixed counterflow systems with emphasis on understanding the effects of hydrodynamics and transport. The resulting scheme yields three zones: (1) a fuel oxidation zone wherein the fuel and oxidizer react to form product as well as a radical R, (e.g., H), (2) a soot/precursor formation zone where the radical R reacts with fuel to form "soot/precursor" S, and (3) a soot/precursor consumption zone where S reacts with the oxidizer to form product. The kinetic scheme, although greatly simplified, allows the coupling between soot inception and flame structure to be assessed. The results yield flame temperature, flame location, and a soot/precursor index S(sub I) as functions of Damkohler number for S formation. The soot/precursor index indicates the amount of S at the boundary of the formation region. The flame temperature indirectly indicates the total amount of S integrated over the formation region because as S is formed less heat release is available. The results show that unlike oxidation reactions, an extinction turning-point behavior does not exist for soot. Instead, the total amount of S slowly decreases with decreasing Damkohler number (increasing strain rate), which is consistent with counterflow flame experiments. When the Lewis number of the radical is decreased from unity, the total S reduces due to reduced residence time for the radical in the soot formation region. Similarly, when the Lewis number of the soot/precursor is increased from unity the amount of S increases for all Damkohler numbers. In addition to studying fuel-air (low stoichiometric mixture fraction) flames, the air-side nitrogen was substituted into the fuel, yielding diluted fuel-oxygen (high stoichiometric mixture fraction) flames with the same flame temperature as the fuel - air flames. The relative flame locations were different however, and, consistent with counterflow flame experiments, this difference was found to dramatically reduce the total amount of S generated because the change in stoichiometric mixture fraction affects residence times, temperatures and concentrations in the soot/precursor formation and consumption zones. Furthermore, while the soot/precursor consumption reaction had a negligible effect on the soot process for fuel-air flames it was very important to diluted fuel - oxygen flames.

A self-regenerable soot sensor with a proton-conductive thin electrolyte and a nanostructured platinum sensing electrode.

PubMed

Lv, Peiling; Ito, Takenori; Oogushi, Akihide; Nakashima, Kensaku; Nagao, Masahiro; Hibino, Takashi

2016-11-18

In recent years, exhaust sensors have become increasingly attractive for use in energy and environmental technologies. Important issues regarding practical applications of these sensors, especially for soot measurements, include the further development of ion-conductive electrolytes and active electrode catalysts for meeting performance and durability requirements. Herein, we design a proton conductor with a high breakdown voltage and a sensing electrode with high sensitivity to electrochemical carbon oxidation, enabling continuous soot monitoring with self-regeneration of the sensor. A Si 0.97 Al 0.03 H x P 2 O 7-δ layer with an excellent balance between proton conductivity and voltage endurance was grown on the surface of a Si 0.97 Al 0.03 O 2-δ substrate by reacting it with liquid H 3 PO 4 at 600 °C. Specific reactivity of the electrochemically formed active oxygen toward soot was accomplished by adding a Pt-impregnated Sn 0.9 In 0.1 H x P 2 O 7-δ catalyst into a Pt sensing electrode. To make the best use of these optimized materials, a unipolar electrochemical device was fabricated by configuring the sensing and counter electrodes on the same surface of the electrolyte layer. The resulting amperometric mode sensor successfully produced a current signal that corresponded to the quantity of soot.

A self-regenerable soot sensor with a proton-conductive thin electrolyte and a nanostructured platinum sensing electrode

PubMed Central

Lv, Peiling; Ito, Takenori; Oogushi, Akihide; Nakashima, Kensaku; Nagao, Masahiro; Hibino, Takashi

2016-01-01

In recent years, exhaust sensors have become increasingly attractive for use in energy and environmental technologies. Important issues regarding practical applications of these sensors, especially for soot measurements, include the further development of ion-conductive electrolytes and active electrode catalysts for meeting performance and durability requirements. Herein, we design a proton conductor with a high breakdown voltage and a sensing electrode with high sensitivity to electrochemical carbon oxidation, enabling continuous soot monitoring with self-regeneration of the sensor. A Si0.97Al0.03HxP2O7-δ layer with an excellent balance between proton conductivity and voltage endurance was grown on the surface of a Si0.97Al0.03O2-δ substrate by reacting it with liquid H3PO4 at 600 °C. Specific reactivity of the electrochemically formed active oxygen toward soot was accomplished by adding a Pt-impregnated Sn0.9In0.1HxP2O7-δ catalyst into a Pt sensing electrode. To make the best use of these optimized materials, a unipolar electrochemical device was fabricated by configuring the sensing and counter electrodes on the same surface of the electrolyte layer. The resulting amperometric mode sensor successfully produced a current signal that corresponded to the quantity of soot. PMID:27857193

A self-regenerable soot sensor with a proton-conductive thin electrolyte and a nanostructured platinum sensing electrode

NASA Astrophysics Data System (ADS)

Lv, Peiling; Ito, Takenori; Oogushi, Akihide; Nakashima, Kensaku; Nagao, Masahiro; Hibino, Takashi

2016-11-01

In recent years, exhaust sensors have become increasingly attractive for use in energy and environmental technologies. Important issues regarding practical applications of these sensors, especially for soot measurements, include the further development of ion-conductive electrolytes and active electrode catalysts for meeting performance and durability requirements. Herein, we design a proton conductor with a high breakdown voltage and a sensing electrode with high sensitivity to electrochemical carbon oxidation, enabling continuous soot monitoring with self-regeneration of the sensor. A Si0.97Al0.03HxP2O7-δ layer with an excellent balance between proton conductivity and voltage endurance was grown on the surface of a Si0.97Al0.03O2-δ substrate by reacting it with liquid H3PO4 at 600 °C. Specific reactivity of the electrochemically formed active oxygen toward soot was accomplished by adding a Pt-impregnated Sn0.9In0.1HxP2O7-δ catalyst into a Pt sensing electrode. To make the best use of these optimized materials, a unipolar electrochemical device was fabricated by configuring the sensing and counter electrodes on the same surface of the electrolyte layer. The resulting amperometric mode sensor successfully produced a current signal that corresponded to the quantity of soot.

Evolution of In-Cylinder Diesel Engine Soot and Emission Characteristics Investigated with Online Aerosol Mass Spectrometry.

PubMed

Malmborg, V B; Eriksson, A C; Shen, M; Nilsson, P; Gallo, Y; Waldheim, B; Martinsson, J; Andersson, Ö; Pagels, J

2017-02-07

To design diesel engines with low environmental impact, it is important to link health and climate-relevant soot (black carbon) emission characteristics to specific combustion conditions. The in-cylinder evolution of soot properties over the combustion cycle and as a function of exhaust gas recirculation (EGR) was investigated in a modern heavy-duty diesel engine. A novel combination of a fast gas-sampling valve and a soot particle aerosol mass spectrometer (SP-AMS) enabled online measurements of the in-cylinder soot chemistry. The results show that EGR reduced the soot formation rate. However, the late cycle soot oxidation rate (soot removal) was reduced even more, and the net effect was increased soot emissions. EGR resulted in an accumulation of polycyclic aromatic hydrocarbons (PAHs) during combustion, and led to increased PAH emissions. We show that mass spectral and optical signatures of the in-cylinder soot and associated low volatility organics change dramatically from the soot formation dominated phase to the soot oxidation dominated phase. These signatures include a class of fullerene carbon clusters that we hypothesize represent less graphitized, C 5 -containing fullerenic (high tortuosity or curved) soot nanostructures arising from decreased combustion temperatures and increased premixing of air and fuel with EGR. Altered soot properties are of key importance when designing emission control strategies such as diesel particulate filters and when introducing novel biofuels.

Simulation on Soot Oxidation with NO2 and O2 in a Diesel Particulate Filter

NASA Astrophysics Data System (ADS)

Yamamoto, Kazuhiro; Satake, Shingo; Yamashita, Hiroshi; Obuchi, Akira; Uchisawa, Junko

Although diesel engines have an advantage of low fuel consumption in comparison with gasoline engines, exhaust gas has more particulate matters (PM) including soot. As one of the key technologies, a diesel particulate filter (DPF) has been developed to reduce PM. When the exhaust gas passes its porous filter wall, the soot particles are trapped. However, the filter would readily be plugged with particles, and the accumulated particles must be removed to prevent filter clogging and a rise in backpressure, which is called filter regeneration process. In this study, we have simulated the flow in the wall-flow DPF using the lattice Boltzmann method. Filters of different length, porosity, and pore size are used. The soot oxidation for filter regeneration process is considered. Especially, the effect of NO2 on the soot oxidation is examined. The reaction rate has been determined by previous experimental data. Results show that, the flow along the filter monolith is roughly uniform, and the large pressure drop across the filter wall is observed. The soot oxidation rate becomes ten times larger when NO2 is added. These are useful information to construct the future regeneration system.

Effect of metal oxides and black carbon (soot) on SO[sub 2]/O[sub 2]/H[sub 2]O reaction systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chughtai, A.R.; Brooks, M.E.; Smith, D.M.

1993-08-01

Particulates of atmospheric interest, including soot, oxidized soot, and oxides of transition metals, [open quotes]fellow travelers[close quotes] in the combustion of solid or liquid fossil fuels, have been examined for their influence on the heterogeneous oxidation of S(IV) to S(VI), both with and without the presence of simulated solar radiation. Under all conditions, MnO[sub 2] has been found to be the most active of the materials in this study. Effectiveness for the oxidation of SO[sub 2] in the presence of oxygen and water vapor decreases in the order: MnO[sub 2] [much gt] V[sub 2]O[sub 5] > CuO > Fe[sub 2]O[submore » 3] > Al[sub 2]O[sub 3] > Soot > TiO[sub 2] = SiO[sub 2] (cab-o-sil) [approximately] ZnO > ozonized soot = blank. The oxidation of SO[sub 2] also was carried out in the presence of soot-MnO[sub 2], soot-V[sub 2]O[sub 5], and soot-Fe[sub 2]O[sub 3] mixtures. The respective sulfate yields were found to be significantly higher than those obtained under similar conditions for the individual substrates. Other combinations, such as MnO[sub 2]/V[sub 2]O[sub 5] and MnO[sub 2]/Fe[sub 2]O[sub 3], yielded sulfate at levels higher than those obtained by any of the transition metal oxides or other oxide mixtures used. The mixing ratio of 1:0.75 (wt/wt) in the MnO[sub 2]/V[sub 2]O[sub 5] mixture was found to be optimum. With this mixture the sulfate yield was nearly twice the amount obtained if only MnO[sub 2] was used and nearly four times the amount if V[sub 2]O[sub 5] was used alone. Extensive analyses of the optimum mixture, to detect any unique identity, were inconclusive. 49 refs., 9 figs.« less

Flammability Parameters of Candles

NASA Astrophysics Data System (ADS)

Balog, Karol; Kobetičová, Hana; Štefko, Tomáš

2017-06-01

The paper deals with the assessment of selected fire safety characteristics of candles. Weight loss of a candle during the burning process, candle burning rate, soot index, heat release rate and yield of carbon oxides were determined. Soot index was determined according to EN 15426: 2007 - Candles - Specification for Sooting Behavior. All samples met the prescribed amount of produced soot. Weight loss, heat release rate and the yield of carbon oxides were determined for one selected sample. While yield of CO increased during the measurement, the yield of CO2 decreased by half in 40 minutes.

Soot loading in a generic gas turbine combustor

NASA Technical Reports Server (NTRS)

Eckerle, W. A.; Rosfjord, T. J.

1987-01-01

Variation in soot loading along the centerline of a generic gas turbine combustor was experimentally investigated. The 12.7-cm dia burner consisted of six sheet-metal louvers. Soot loading along the burner length was quantified by acquiring measurements first at the exit of the full-length combustor and then at upstream stations by sequential removal of liner louvers to shorten the burner length. Alteration of the flow field approaching removed louvers, maintaining a constant liner pressure drop. Burner exhaust flow was sampled at the burner centerline to determine soot mass concentration and smoke number. Characteristic particle size and number density, transmissivity of the exhaust flow, and local radiation from luminous soot particles in the exhaust flow were determined by optical techniques. Four test fuels were burned at three fuel-air ratios to determine fuel chemical property and flow temperature influences. Data were acquired at two combustor pressures. Particulate concentration data indicated a strong oxidation mechanism in the combustor secondary zone, though the oxidation was significantly affected by flow temperature. Soot production was directly related to fuel smoke point. Less soot production and lower secondary-zone oxidation rates were observed at reduced combustor pressure.

Modeling Soot Oxidation and Gasification with Bayesian Statistics

DOE PAGES

Josephson, Alexander J.; Gaffin, Neal D.; Smith, Sean T.; ...

2017-08-22

This paper presents a statistical method for model calibration using data collected from literature. The method is used to calibrate parameters for global models of soot consumption in combustion systems. This consumption is broken into two different submodels: first for oxidation where soot particles are attacked by certain oxidizing agents; second for gasification where soot particles are attacked by H 2O or CO 2 molecules. Rate data were collected from 19 studies in the literature and evaluated using Bayesian statistics to calibrate the model parameters. Bayesian statistics are valued in their ability to quantify uncertainty in modeling. The calibrated consumptionmore » model with quantified uncertainty is presented here along with a discussion of associated implications. The oxidation results are found to be consistent with previous studies. Significant variation is found in the CO 2 gasification rates.« less

Modeling Soot Oxidation and Gasification with Bayesian Statistics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Josephson, Alexander J.; Gaffin, Neal D.; Smith, Sean T.

This paper presents a statistical method for model calibration using data collected from literature. The method is used to calibrate parameters for global models of soot consumption in combustion systems. This consumption is broken into two different submodels: first for oxidation where soot particles are attacked by certain oxidizing agents; second for gasification where soot particles are attacked by H 2O or CO 2 molecules. Rate data were collected from 19 studies in the literature and evaluated using Bayesian statistics to calibrate the model parameters. Bayesian statistics are valued in their ability to quantify uncertainty in modeling. The calibrated consumptionmore » model with quantified uncertainty is presented here along with a discussion of associated implications. The oxidation results are found to be consistent with previous studies. Significant variation is found in the CO 2 gasification rates.« less

The effect of soot on ammonium nitrate species and NO2 selective catalytic reduction over Cu-zeolite catalyst-coated particulate filter.

PubMed

Mihai, Oana; Tamm, Stefanie; Stenfeldt, Marie; Olsson, Louise

2016-02-28

A selective catalytic reduction (SCR)-coated particulate filter was evaluated by means of dynamic tests performed using NH3, NO2, O2 and H2O. The reactions were examined both prior to and after soot removal in order to study the effect of soot on ammonium nitrate formation and decomposition, ammonia storage and NO2 SCR. A slightly larger ammonia storage capacity was observed when soot was present in the sample, which indicated that small amounts of ammonia can adsorb on the soot. Feeding of NO2 and NH3 in the presence of O2 and H2O at low temperature (150, 175 and 200°C) leads to a large formation of ammonium nitrate species and during the subsequent temperature ramp using H2O and argon, a production of nitrous oxides was observed. The N2O formation is often related to ammonium nitrate decomposition, and our results showed that the N2O formation was clearly decreased by the presence of soot. We therefore propose that in the presence of soot, there are fewer ammonium nitrate species on the surface due to the interactions with the soot. Indeed, we do observe CO2 production during the reaction conditions also at 150°C, which shows that there is a reaction with these species and soot. In addition, the conversion of NOx due to NO2 SCR was significantly enhanced in the presence of soot; we attribute this to the smaller amount of ammonium nitrate species present in the experiments where soot is available since it is well known that ammonium nitrate formation is a major problem at low temperature due to the blocking of the catalytic sites. Further, a scanning electron microscopy analysis of the soot particles shows that they are about 30-40 nm and are therefore too large to enter the pores of the zeolites. There are likely CuxOy or other copper species available on the outside of the zeolite crystallites, which could have been enhanced due to the hydrothermal treatment at 850°C of the SCR-coated filter prior to the soot loading. We therefore propose that soot is interacting with the ammonium nitrate species on the CuxOy or other copper species on the surface of the zeolite particles, which reduces the ammonium nitrate blocking of the catalyst and thereby results in higher NO2 SCR activity. © 2016 The Author(s).

The effect of oxygen enrichment on soot formation and thermal radiation in turbulent, non-premixed methane flames

DOE PAGES

Shaddix, Christopher R.; Williams, Timothy C.

2016-07-12

Non-premixed oxy-fuel combustion of natural gas is used in industrial applications where high-intensity heat is required, such as glass manufacturing and metal forging and shaping. In these applications, the high flame temperatures achieved by oxy-fuel combustion increase radiative heat transfer to the surfaces of interest and soot formation within the flame is desired for further augmentation of radiation. However, the high cost of cryogenic air separation has limited the penetration of oxy-fuel combustion technologies. New approaches to air separation are being developed that may reduce oxygen production costs, but only for intermediate levels of oxygen enrichment of air. To determinemore » the influence of oxygen enrichment on soot formation and radiation, we developed a non-premixed coannular burner in which oxygen concentrations and oxidizer flow rates can be independently varied, to distinguish the effects of turbulent mixing intensity from oxygen enrichment on soot formation and flame radiation. Local radiation intensities, soot concentrations, and soot temperatures have been measured using a thin-film thermopile, planar laser-induced incandescence (LII), and two-color imaging pyrometry, respectively. The measurements show that soot formation increases as the oxygen concentration decreases from 100% to 50%, helping to moderate a decrease in overall flame radiation. An increase in turbulence intensity has a marked effect on flame height, soot formation and thermal radiation, leading to decreases in all of these. The soot temperature decreases with a decrease in the oxygen concentration and increases with an increase in turbulent mixing intensity. Altogether, the results suggest that properly designed oxygen-enriched burners that enhance soot formation for intermediate levels of oxygen purity may be able to achieve thermal radiation intensities as high as 85% of traditional oxy-fuel burners utilizing high-purity oxygen.« less

The effect of oxygen enrichment on soot formation and thermal radiation in turbulent, non-premixed methane flames

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shaddix, Christopher R.; Williams, Timothy C.

Non-premixed oxy-fuel combustion of natural gas is used in industrial applications where high-intensity heat is required, such as glass manufacturing and metal forging and shaping. In these applications, the high flame temperatures achieved by oxy-fuel combustion increase radiative heat transfer to the surfaces of interest and soot formation within the flame is desired for further augmentation of radiation. However, the high cost of cryogenic air separation has limited the penetration of oxy-fuel combustion technologies. New approaches to air separation are being developed that may reduce oxygen production costs, but only for intermediate levels of oxygen enrichment of air. To determinemore » the influence of oxygen enrichment on soot formation and radiation, we developed a non-premixed coannular burner in which oxygen concentrations and oxidizer flow rates can be independently varied, to distinguish the effects of turbulent mixing intensity from oxygen enrichment on soot formation and flame radiation. Local radiation intensities, soot concentrations, and soot temperatures have been measured using a thin-film thermopile, planar laser-induced incandescence (LII), and two-color imaging pyrometry, respectively. The measurements show that soot formation increases as the oxygen concentration decreases from 100% to 50%, helping to moderate a decrease in overall flame radiation. An increase in turbulence intensity has a marked effect on flame height, soot formation and thermal radiation, leading to decreases in all of these. The soot temperature decreases with a decrease in the oxygen concentration and increases with an increase in turbulent mixing intensity. Altogether, the results suggest that properly designed oxygen-enriched burners that enhance soot formation for intermediate levels of oxygen purity may be able to achieve thermal radiation intensities as high as 85% of traditional oxy-fuel burners utilizing high-purity oxygen.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

John E. Dec; Peter L. Kelly-Zion

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 andmore » 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.« less

Effects of Structure and Hydrodynamics on the Sooting Behavior of Spherical Microgravity Diffusion Flames

NASA Technical Reports Server (NTRS)

Sunderland, P. B.; Axelbaum, Richard L.; Urban, D. L.

2000-01-01

We have examined the sooting behavior of spherical microgravity diffusion flames burning ethylene at atmospheric pressure in the NASA Glenn 2.2-second drop tower. In a novel application of microgravity, spherical flames allowed convection across the flame to be either from fuel to oxidizer or from oxidizer to fuel. Thus, microgravity flames are uniquely capable of allowing independent variation of convection direction across the flame and stoichiometric mixture fraction, Z(sub st). This allowed us to determine the dominant mechanism responsible for the phenomenon of permanently-blue diffusion flames -- flames that remain blue as strain rate approaches zero. Stoichiometric mixture fraction was varied by changing inert concentrations such that adiabatic flame temperature did not change. At low and high Z(sub st) nitrogen was supplied with the oxidizer and the fuel, respectively. For the present flames, structure (Z(sub st)) was found to have a profound effect on soot production. Soot-free conditions were observed at high Z(sub st) (Z(sub st) = 0.78) and sooting conditions were observed at low Z(sub st) (Z(sub st) = 0.064) regardless of the direction of convection. Convection direction was found to have a lesser impact on soot inception, with formation being suppressed when convection at the flame sheet was directed towards the oxidizer.

Morphology and nano-structure analysis of soot particles sampled from high pressure diesel jet flames under diesel-like conditions

NASA Astrophysics Data System (ADS)

Jiang, Hao; Li, Tie; Wang, Yifeng; He, Pengfei

2018-04-01

Soot particles emitted from diesel engines have a significant impact on the atmospheric environment. Detailed understanding of soot formation and oxidation processes is helpful for reducing the pollution of soot particles, which requires information such as the size and nano-structure parameters of the soot primary particles sampled in a high-temperature and high-pressure diesel jet flame. Based on the thermophoretic principle, a novel sampling probe minimally disturbing the diesel jet flame in a constant volume combustion vessel is developed for analysing soot particles. The injected quantity of diesel fuel is less than 10 mg, and the soot particles sampled by carriers with a transmission electron microscope (TEM) grid and lacey TEM grid can be used to analyse the morphologies of soot aggregates and the nano-structure of the soot primary particles, respectively. When the quantity of diesel fuel is more than 10 mg, in order to avoid burning-off of the carriers in higher temperature and pressure conditions, single-crystal silicon chips are employed. Ultrasonic oscillations and alcohol extraction are then implemented to obtain high quality soot samples for observation using a high-resolution transmission electron microscope. An in-house Matlab-based code is developed to extract the nano-structure parameters of the soot particles. A complete sampling and analysis procedure of the soot particles is provided to study the formation and oxidation mechanism of soot.

Water interaction with hydrophobic and hydrophilic soot particles.

PubMed

Popovicheva, Olga; Persiantseva, Natalia M; Shonija, Natalia K; DeMott, Paul; Koehler, Kirsten; Petters, Markus; Kreidenweis, Sonia; Tishkova, Victoria; Demirdjian, Benjamin; Suzanne, Jean

2008-05-07

The interaction of water with laboratory soots possessing a range of properties relevant for atmospheric studies is examined by two complementary methods: gravimetrical measurement of water uptake coupled with chemical composition and porosity analysis and HTDMA (humidified tandem differential mobility analyzer) inference of water uptake accompanied by separate TEM (transmission electron microscopy) analysis of single particles. The first method clarifies the mechanism of water uptake for bulk soot and allows the classification of soot with respect to its hygroscopicity. The second method highlights the dependence of the soot aerosol growth factor on relative humidity (RH) for quasi-monodisperse particles. Hydrophobic and hydrophilic soot are qualitatively defined by their water uptake and surface polarity: laboratory soot particles are thus classified from very hydrophobic to very hydrophilic. Thermal soot particles produced from natural gas combustion are classified as hydrophobic with a surface of low polarity since water is found to cover only half of the surface. Graphitized thermal soot particles are proposed for comparison as extremely hydrophobic and of very low surface polarity. Soot particles produced from laboratory flame of TC1 aviation kerosene are less hydrophobic, with their entire surface being available for statistical monolayer water coverage at RH approximately 10%. Porosity measurements suggest that, initially, much of this surface water resides within micropores. Consequently, the growth factor increase of these particles to 1.07 at RH > 80% is attributed to irreversible swelling that accompanies water uptake. Hysteresis of adsorption/desorption cycles strongly supports this conclusion. In contrast, aircraft engine soot, produced from burning TC1 kerosene in a gas turbine engine combustor, has an extremely hydrophilic surface of high polarity. Due to the presence of water soluble organic and inorganic material it can be covered by many water layers even below water saturation conditions. This soot demonstrates a gradual diameter growth factor (D(wet)/D(dry)) increase up to 1.22 at 93% relative humidity, most likely due to the presence of single particles with water soluble material heterogeneously distributed over their surface.

Effects of self-absorption on simultaneous estimation of temperature distribution and concentration fields of soot and metal-oxide nanoparticles in nanofluid fuel flames using a spectrometer

NASA Astrophysics Data System (ADS)

Liu, Guannan; Liu, Dong

2018-06-01

An improved inverse reconstruction model with consideration of self-absorption effect for the temperature distribution and concentration fields of soot and metal-oxide nanoparticles in nanofluid fuel flames was proposed based on the flame emission spectrometry. The effects of self-absorption on the temperature profile and concentration fields were investigated for various measurement errors, flame optical thicknesses and detecting lines numbers. The model neglecting the self-absorption caused serious reconstruction errors especially in the nanofluid fuel flames with large optical thicknesses, while the improved model was used to successfully recover the temperature distribution and concentration fields of soot and metal-oxide nanoparticles for the flames regardless of the optical thickness. Through increasing detecting lines number, the reconstruction accuracy can be greatly improved due to more flame emission information received by the spectrometer. With the adequate detecting lines number, the estimations for the temperature distribution and concentration fields of soot and metal-oxide nanoparticles in flames with large optical thicknesses were still satisfying even from the noisy radiation intensities with signal to noise ratio (SNR) as low as 46 dB. The results showed that the improved reconstruction model was effective and robust to concurrently retrieve the temperature distribution and volume fraction fields of soot and metal-oxide nanoparticles for the exact and noisy data in nanofluid fuel sooting flames with different optical thicknesses.

Interactions of SO{sub x} and NO{sub x} with soot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, D.M.; Chughtai, A.R.; Konowalchuk, B.K.

1996-10-01

Studies of the adsorption of oxides of sulfur and nitrogen, and their coadsorption, on black carbon in the form of n-hexane soot have been carried out by microgravimetry, EPR and FTIR spectroscopy over a wide range of experimental conditions. The mechanisms of adsorption of O{sub 2} and NO{sub 2} are entirely different, as reflected by adsorption isotherms, the behavior of carbon`s unpaired electrons, the spectral features of surface species formed, mass changes during adsorption-desorption cycles, and an essential lack of competition for surface sites. Significant effects of temperature, water, SO{sub 2} and NO{sub 2} concentration, O{sub 2}, simulated solar radiation,more » and the presence of trace metals, have been observed and interpreted.« less

Characterization of the particulate emissions from the BP Deepwater Horizon surface oil burns.

PubMed

Gullett, Brian K; Hays, Michael D; Tabor, Dennis; Wal, Randy Vander

2016-06-15

Sampling of the smoke plumes from the BP Deepwater Horizon surface oil burns led to the unintentional collection of soot particles on the sail of an instrument-bearing, tethered aerostat. This first-ever plume sampling from oil burned at an actual spill provided an opportunistic sample from which to characterize the particles' chemical properties for polycyclic aromatic hydrocarbons (PAHs), organic carbon, elemental carbon, metals, and polychlorinated dibenzodioxins/dibenzofurans (PCDDs/PCDFs) and physical properties for size and nanostructure. Thermal-optical analyses indicated that the particulate matter was 93% carbon with 82% being refractory elemental carbon. PAHs accounted for roughly 68μg/g of the PM filter mass and 5mg/kg oil burned, much lower than earlier laboratory based studies. Microscopy indicated that the soot is distinct from more common soot by its aggregate size, primary particle size, and nanostructure. PM-bound metals were largely unremarkable but PCDD/PCDF formation was observed, contrary to other's findings. Levels of lighter PCDD/PCDF and PAH compounds were reduced compared to historical samples, possibly due to volatilization or photo-oxidation. Published by Elsevier Ltd.

Revealing the role of oxidation state in interaction between nitro/amino-derived particulate matter and blood proteins

PubMed Central

Liu, Zhen; Li, Ping; Bian, Weiwei; Yu, Jingkai; Zhan, Jinhua

2016-01-01

Surface oxidation states of ultrafine particulate matter can influence the proinflammatory responses and reactive oxygen species levels in tissue. Surface active species of vehicle-emission soot can serve as electron transfer-mediators in mitochondrion. Revealing the role of surface oxidation state in particles-proteins interaction will promote the understanding on metabolism and toxicity. Here, the surface oxidation state was modeled by nitro/amino ligands on nanoparticles, the interaction with blood proteins were evaluated by capillary electrophoresis quantitatively. The nitro shown larger affinity than amino. On the other hand, the affinity to hemoglobin is 103 times larger than that to BSA. Further, molecular docking indicated the difference of binding intensity were mainly determined by hydrophobic forces and hydrogen bonds. These will deepen the quantitative understanding of protein-nanoparticles interaction from the perspective of surface chemical state. PMID:27181651

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

NASA Astrophysics Data System (ADS)

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.

Conductivity for soot sensing: possibilities and limitations.

PubMed

Grob, Benedikt; Schmid, Johannes; Ivleva, Natalia P; Niessner, Reinhard

2012-04-17

In this study we summarize the possibilities and limitations of a conductometric measurement principle for soot sensing. The electrical conductivity of different carbon blacks (FW 200, lamp black 101, Printex 30, Printex U, Printex XE2, special black 4, and special black 6), spark discharge soot (GfG), and graphite powder was measured by a van der Pauw arrangement. Additionally the influence of inorganic admixtures on the conductivity of carbonaceous materials was proven to follow the percolation theory. Structural and oxidation characteristics obtained with Raman microspectroscopy and temperature programmed oxidation, respectively, were correlated with the electrical conductivity data. Moreover, a thermophoretic precipitator has been applied to deposit soot particles from the exhaust stream between interdigital electrodes. This combines a controlled and size independent particle collection method with the conductivity measurement principle. A test vehicle was equipped with the AVL Micro Soot Sensor (photoacoustic soot sensor) to prove the conductometric sensor principle with an independent and reliable technique. Our results demonstrate promising potential of the conductometric sensor for on-board particle diagnostic. Furthermore this sensor can be applied as a simple, rapid, and cheap analytical tool for characterization of soot structure.

Experimental and theoretical study of diesel soot reactivity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marcuccilli, F; Gilot, P.; Stanmore, B.

1994-12-31

In order to provide data for modelling the performance of a regenerative soot filter, a study of the oxidation kinetics of diesel soot in the temperature range from 600 C to 800 C was undertaken. Isothermal burning rates at a number of temperatures were measured in rectangular soot beds within a thermobalance. The technique was easy to use, but the combustion rate was found to depend on bed mass. The oxidation process was thus limited by mass transfer effects. A two-dimensional mathematical model of oxygen transfer was developed to extract the true kinetic rates from experimental data. The two-dimensional approachmore » was required because significant oxygen depletion occurred along both axes. Using assumed kinetic rates, oxygen concentration profiles in the gas phase above the bed and within the bed were calculated. The true kinetics at a number of temperatures were, then established by matching predicted oxygen consumption with measured consumption. Application of the model required values of the effective diffusion coefficient for oxygen within the bed. Accordingly, the structure and properties of the soot aggregates were determined. A supplements study was carried out to identify the appropriate primary reaction products. The measured kinetic rates were then used in a simpler, monodimensional model to evaluate the mean oxygen mass transfer coefficients to the surface of the bed. The results show that burning below about 730 C is in regime 1 and can be described by K = 6.9 {times} 10{sup 12} exp ({minus}207,000/RT) (s{sup {minus}1}) with R = 8.314 J/mol {times} K. Above, 730 C, there is a decrease in apparent activation energy, probably due to thermal ``annealing,`` which changes the microstructure of the carbon. As a result, the inherent reactivity declines and/or the bed becomes less accessible to oxygen.« less

Uptake of HNO3 on aviation kerosene and aircraft engine soot: influences of H2O or/and H2SO4.

PubMed

Loukhovitskaya, Ekaterina E; Talukdar, Ranajit K; Ravishankara, A R

2013-06-13

The uptake of HNO3 on aviation kerosene soot (TC-1 soot) was studied in the absence and presence of water vapor at 295 and 243 K. The influence of H2SO4 coating of the TC-1 soot surface on HNO3 uptake was also investigated. Only reversible uptake of HNO3 was observed. HONO and NO2, potential products of reactive uptake of HNO3, were not observed under any conditions studied here. The uptake of nitric acid increased slightly with relative humidity (RH). Coating of the TC-1 soot surface with sulfuric acid decreased the uptake of HNO3 and did not lead to displacement of H2SO4 from the soot surface. A limited set of measurements was carried out on soot generated by aircraft engine combustor (E-soot) with results similar to those on TC-1 soot. The influence of water on HNO3 uptake on E-soot appeared to be more pronounced than on TC-1 soot. Our results suggest that HNO3 loss in the upper troposphere due to soot is not significant except perhaps in aircraft exhaust plumes. Our results also suggest that HNO3 is not converted to either NO2 or HONO upon its uptake on soot in the atmosphere.

A unified intermediate and mechanism for soot combustion on potassium-supported oxides

PubMed Central

Li, Qian; Wang, Xiao; Xin, Ying; Zhang, Zhaoliang; Zhang, Yexin; Hao, Ce; Meng, Ming; Zheng, Lirong; Zheng, Lei

2014-01-01

The soot combustion mechanism over potassium-supported oxides (MgO, CeO2 and ZrO2) was studied to clarify the active sites and discover unified reaction intermediates in this typical gas-solid-solid catalytic reaction. The catalytically active sites were identified as free K+ rather than K2CO3, which can activate gaseous oxygen. The active oxygen spills over to soot and forms a common intermediate, ketene, before it was further oxidized into the end product CO2. The existence of ketene species was confirmed by density functional theory (DFT) calculations. The oxygen spillover mechanism is proposed, which is explained as an electron transfer from soot to gaseous oxygen through the active K+ sites. The latter mechanism is confirmed for the first time since it was put forward in 1950, not only by ultraviolet photoelectron spectroscopy (UPS) results but also by semi-empirical theoretical calculations. PMID:24740213

Distinct oxidative stabilities of char versus soot black carbon: Implications for quantification and environmental recalcitrance

NASA Astrophysics Data System (ADS)

Elmquist, Marie; Cornelissen, Gerard; Kukulska, Zofia; Gustafsson, Örjan

2006-06-01

Sequestration in sediments of black carbon (BC) from vegetation fires and fuel combustion may constitute a significant sink of otherwise rapidly cycling carbon from the atmosphere-biosphere cycle. It also has the potential to provide a historical record of atmospheric BC loadings. Previous treatments of BC as one homogeneous entity are being replaced with the growing awareness of a BC combustion continuum, a range spanning from slightly charred biomass to soot and graphite. Here the relative recalcitrance of different BC forms is evaluated, and implications for both BC quantification and environmental stability are considered. The stabilities of four BC reference materials against thermal oxidation in air were quite distinct with T50%BC values (i.e., the temperature where 50% BC remained in the residue) of 444°C (diesel soot-BC), 388°C (n-hexane soot-BC), 338°C (wood char-BC), and 266°C (grass char-BC). The implications for BC quantification have been illustrated for a thermal oxidation (the CTO-375) method commonly applied to study BC in sediments. This technique measured BC:TOC ratios of 78.3 ± 1.3% for the diesel soot-BC and 45.3 ± 6.1% for n-hexane soot-BC, whereas no CTO375-BC was detected for the two analyzed char-BC materials. The greater lability of char-BC compared to soot-BC likely reflects higher accessibility to internal microporosity in char-BC, facilitating internal O2 transfer. Decreasing the temperature cutoff below 375°C to also include char-BC is not possible as thermograms of nonpyrogenic reference materials indicated that such material would then be artifactually quantified as BC. The presence of mineral oxides in the sediment matrix may lead to a catalytically mediated lowering of the activation energy for soot-BC oxidation but not for char-BC or nonpyrogenic organic material. Several recent studies combine to challenge the proposition of complete recalcitrance of BC. Particularly, the thermal lability of char-BC from grassland fires deserves further attention in order to improve the understanding of BC in the global carbon cycle.

Effects of soot-induced snow albedo change on snowpack and hydrological cycle in western U.S. based on WRF chemistry and regional climate simulations

NASA Astrophysics Data System (ADS)

Qian, Y.; Gustafson, W. I.; Leung, R.; Ghan, S. J.

2008-12-01

Radiative forcing induced by soot on snow is an important anthropogenic forcing affecting the global climate. In this study we simulated the deposition of soot aerosol on snow and the resulting impact on snowpack and the hydrological cycle in the western United States. A yearlong simulation was performed using the chemistry version of the Weather Research and Forecasting model (WRF-Chem) to determine the soot deposition, followed by three simulations using WRF in meteorology-only mode, with and without the soot-induced snow albedo perturbations. The chemistry simulation shows large spatial variability in soot deposition that reflects the localized emissions and the influence of the complex terrain. The soot-induced snow albedo perturbations increase the surface net solar radiation flux during late winter to early spring, increase the surface air temperature, and reduce the snow accumulation and spring snowmelt. These effects are stronger over the central Rockies and southern Alberta, where soot deposition and snowpack overlap the most. The indirect forcing of soot accelerates snowmelt and alters stream flows, including a trend toward earlier melt dates in the western United States. The soot-induced albedo reduction initiates a positive feedback process whereby dirty snow absorbs more solar radiation, heating the surface and warming the air. This warming causes reduced snow depth and fraction, which further reduces the regional surface albedo for the snow covered regions. For a doubled snow albedo perturbation, the change to surface energy and temperature is around 50-80%, however, snowpack reduction is nonlinearly accelerated.

Effects of soot-induced snow albedo change on snowpack and hydrological cycle in western United States based on Weather Research and Forecasting chemistry and regional climate simulations

NASA Astrophysics Data System (ADS)

Qian, Yun; Gustafson, William I.; Leung, L. Ruby; Ghan, Steven J.

2009-02-01

Radiative forcing induced by soot on snow is an important anthropogenic forcing affecting the global climate. In this study we simulated the deposition of soot aerosol on snow and the resulting impact on snowpack and the hydrological cycle in the western United States. A year-long simulation was performed using the chemistry version of the Weather Research and Forecasting model (WRF-Chem) to determine the soot deposition, followed by three simulations using WRF in meteorology-only mode, with and without the soot-induced snow albedo perturbations. The chemistry simulation shows large spatial variability in soot deposition that reflects the localized emissions and the influence of the complex terrain. The soot-induced snow albedo perturbations increase the surface net solar radiation flux during late winter to early spring, increase the surface air temperature, and reduce the snow accumulation and spring snowmelt. These effects are stronger over the central Rockies and southern Alberta, where soot deposition and snowpack overlap the most. The indirect forcing of soot accelerates snowmelt and alters stream flows, including a trend toward earlier melt dates in the western United States. The soot-induced albedo reduction initiates a positive feedback process whereby dirty snow absorbs more solar radiation, heating the surface and warming the air. This warming causes reduced snow depth and fraction, which further reduces the regional surface albedo for the snow-covered regions. For a doubled snow albedo perturbation, the change to surface energy and temperature is around 50-80%; however, snowpack reduction is nonlinearly accelerated.

Light changes the atmospheric reactivity of soot

PubMed Central

Monge, Maria Eugenia; D’Anna, Barbara; Mazri, Linda; Giroir-Fendler, Anne; Ammann, Markus; Donaldson, D. J.; George, Christian

2010-01-01

Soot particles produced by incomplete combustion processes are one of the major components of urban air pollution. Chemistry at their surfaces lead to the heterogeneous conversion of several key trace gases; for example NO2 interacts with soot and is converted into HONO, which rapidly photodissociates to form OH in the troposphere. In the dark, soot surfaces are rapidly deactivated under atmospheric conditions, leading to the current understanding that soot chemistry affects tropospheric chemical composition only in a minor way. We demonstrate here that the conversion of NO2 to HONO on soot particles is drastically enhanced in the presence of artificial solar radiation, and leads to persistent reactivity over long periods. Soot photochemistry may therefore be a key player in urban air pollution. PMID:20080580

Optical and probe determination of soot concentrations in a model gas turbine combustor

NASA Technical Reports Server (NTRS)

Eckerle, W. A.; Rosfjord, T. J.

1986-01-01

An experimental program was conducted to track the variation in soot loading in a generic gas turbine combustor. The burner is a 12.7-cm dia cylindrical device consisting of six sheet-metal louvers. Determination of soot loading along the burner length is achieved by measurement at the exit of the combustor and then at upstream stations by sequential removal of liner louvers to shorten burner length. Alteration of the flow field approaching and within the shortened burners is minimized by bypassing flow in order to maintain a constant linear pressure drop. The burner exhaust flow is sampled at the burner centerline to determine soot mass concentration and smoke number. Characteristic particle size and number density, transmissivity of the exhaust flow, and local radiation from luminous soot particles in the exhaust are determined by optical techniques. Four test fuels are burned at three fuel-air ratios to determine fuel chemical property and flow temperature influences. Particulate concentration data indicate a strong oxidation mechanism in the combustor secondary zone, though the oxidation is significantly affected by flow temperature. Soot production is directly related to fuel smoke point.

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

PubMed

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.

Chemical composition and heterogeneous reactivity of soot generated in the combustion of diesel and GTL (Gas-to-Liquid) fuels and amorphous carbon Printex U with NO2 and CF3COOH gases

NASA Astrophysics Data System (ADS)

Tapia, A.; Salgado, S.; Martín, P.; Villanueva, F.; García-Contreras, R.; Cabañas, B.

2018-03-01

The heterogeneous reactions of nitrogen dioxide (NO2) and trifluoroacetic acid (CF3COOH) with soot produced by diesel and GTL (gas-to-liquid) fuels were investigated using a Knudsen flow reactor with mass spectrometry as a detection system for gas phase species. Soot was generated with a 4 cylinder diesel engine working under steady-state like urban operation mode. Heterogeneous reaction of the mentioned gases with a commercial carbon, Printex U, used as reference, was also analyzed. The initial and the steady-state uptake coefficients, γ0 and γss, respectively, were measured indicating that GTL soot reacts faster than diesel soot and Printex U carbon for NO2 gas reactant. According to the number of reacted molecules on the surface, Printex U soot presents more reducing sites than diesel and GTL soot. Initial uptake coefficients for GTL and diesel soot for the reaction with CF3COOH gas reactant are very similar and no clear conclusions can be obtained related to the initial reactivity. The number of reacted molecules calculated for CF3COOH reactions shows values two orders of magnitude higher than the corresponding to NO2 reactions, indicating a greater presence of basic functionalities in the soot surfaces. More information of the surface composition has been obtained using Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) before and after the reaction of soot samples with gas reactants. As conclusion, the interface of diesel and GTL soot before reaction mainly consists of polycyclic aromatic hydrocarbons (PAHs), nitro-compounds as well as ether functionalities. After reaction with gas reactant, it was observed that PAHs and nitro-compounds remain on the soot surface and new spectral bands such as carbonyl groups (carboxylic acids, aldehydes, esters and ketones) are observed. Physical properties of soot from both fuels studied such as BET surface isotherm and SEM analysis were also developed and related to the observed reactivity.

Estimating soot emissions from an elevated flare

NASA Astrophysics Data System (ADS)

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.

Chemical characterization of diesel and hydrotreated vegetable oil (HVO) soot after reactive gas probing using diffuse reflectance FTIR spectroscopy (DRIFTS).

PubMed

Tapia, A; Salgado, M S; Martín, M P; Rodríguez-Fernández, J; Rossi, M J; Cabañas, B

2017-03-01

A chemical characterization of diesel and hydrotreated vegetable oil (HVO) soot has been developed using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) before and after the reaction with different probe gases. Samples were generated under combustion conditions corresponding to an urban operation mode of a diesel engine and were reacted with probe gas-phase molecules in a Knudsen flow reactor. Specifically, NH 2 OH, O 3 and NO 2 were used as reactants (probes) and selected according to their reactivities towards specific functional groups on the sample surface. Samples of previously ground soot were diluted with KBr and were introduced in a DRIFTS accessory. A comparison between unreacted and reacted soot samples was made in order to establish chemical changes on the soot surface upon reaction. It was concluded that the interface of diesel and HVO soot before reaction mainly consists polycyclic aromatic hydrocarbons, nitro and carbonyl compounds, as well as ether functionalities. The main difference between both soot samples was observed in the band of the C=O groups that in diesel soot was observed at 1719 cm -1 but not in HVO soot. After reaction with probe gases, it was found that nitro compounds remain on the soot surface, that the degree of unsaturation decreases for reacted samples, and that new spectral bands such as hydroxyl groups are observed.

Durable superhydrophobic carbon soot coatings for sensor applications

NASA Astrophysics Data System (ADS)

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.

Effect of diesel oxidation catalysts on the diesel particulate filter regeneration process.

PubMed

Lizarraga, Leonardo; Souentie, Stamatios; Boreave, Antoinette; George, Christian; D'Anna, Barbara; Vernoux, Philippe

2011-12-15

A Diesel Particulate Filter (DPF) regeneration process was investigated during aftertreatment exhaust of a simulated diesel engine under the influence of a Diesel Oxidation Catalyst (DOC). Aerosol mass spectrometry analysis showed that the presence of the DOC decreases the Organic Carbon (OC) fraction adsorbed to soot particles. The activation energy values determined for soot nanoparticles oxidation were 97 ± 5 and 101 ± 8 kJ mol(-1) with and without the DOC, respectively; suggesting that the DOC does not facilitate elementary carbon oxidation. The minimum temperature necessary for DPF regeneration was strongly affected by the presence of the DOC in the aftertreatment. The conversion of NO to NO(2) inside the DOC induced the DPF regeneration process at a lower temperature than O(2) (ΔT = 30 K). Also, it was verified that the OC fraction, which decreases in the presence of the DOC, plays an important role to ignite soot combustion.

[Catalytic performance of Ce/Zr series catalysts on soot combustion].

PubMed

Zhu, Ling; Wang, Xue-Zhong; Hao, Zheng-Ping

2005-09-01

Catalytic performances of Ce/Zr series catalysts (Ce(x)Zr(1-x)O2) on soot combustion and the influence of feed gas were investigated by TG and TPO. The catalytic activity is high, and affects by the Ce/Zr ratio. The concentration of O2 affects the speed-limited step during the process of soot combustion. H2O showed no effect on the catalytic activity for soot combustion on Ce(0.5)Zr(0.5)O2. NO could promote soot combustion by presenting NO2, a more powerful oxidant than O2, and the ignition temperature of soot decreased 30 degrees C. Results of TG and TPO show that the beta species oxygen on the catalyst take part in the combustion process.

Laser-diagnostic mapping of temperature and soot statistics in a 2-m diameter turbulent pool fire

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kearney, Sean P.; Grasser, Thomas W.

We present spatial profiles of temperature and soot-volume-fraction statistics from a sooting 2-m base diameter turbulent pool fire, burning a 10%-toluene / 90%-methanol fuel mixture. Dual-pump coherent anti-Stokes Raman scattering and laser-induced incandescence are utilized to obtain radial profiles of temperature and soot probability density functions (pdf) as well as estimates of temperature/soot joint statistics at three vertical heights above the surface of the methanol/toluene fuel pool. Results are presented both in the fuel vapor-dome region at ¼ base diameter and in the actively burning region at ½ and ¾ diameters above the fuel surface. The spatial evolution of themore » soot and temperature pdfs is discussed and profiles of the temperature and soot mean and rms statistics are provided. Joint temperature/soot statistics are presented as spatially resolved conditional averages across the fire plume, and in terms of a joint pdf obtained by including measurements from multiple spatial locations.« less

Laser-diagnostic mapping of temperature and soot statistics in a 2-m diameter turbulent pool fire

DOE PAGES

Kearney, Sean P.; Grasser, Thomas W.

2017-08-10

We present spatial profiles of temperature and soot-volume-fraction statistics from a sooting 2-m base diameter turbulent pool fire, burning a 10%-toluene / 90%-methanol fuel mixture. Dual-pump coherent anti-Stokes Raman scattering and laser-induced incandescence are utilized to obtain radial profiles of temperature and soot probability density functions (pdf) as well as estimates of temperature/soot joint statistics at three vertical heights above the surface of the methanol/toluene fuel pool. Results are presented both in the fuel vapor-dome region at ¼ base diameter and in the actively burning region at ½ and ¾ diameters above the fuel surface. The spatial evolution of themore » soot and temperature pdfs is discussed and profiles of the temperature and soot mean and rms statistics are provided. Joint temperature/soot statistics are presented as spatially resolved conditional averages across the fire plume, and in terms of a joint pdf obtained by including measurements from multiple spatial locations.« less

Soot Formation in Laminar Premixed Ethylene/Air Flames at Atmospheric Pressure. Appendix G

NASA Technical Reports Server (NTRS)

Xu, F.; Sunderland, P. B.; Faeth, G. M.; Urban, D. L. (Technical Monitor)

2001-01-01

Soot formation was studied within laminar premixed ethylene/air flames (C/O ratios of 0.78-0.98) stabilized on a flat-flame burner operating at atmospheric pressure. Measurements included soot volume fractions by both laser extinction and gravimetric methods, temperatures by multiline emission, soot structure by thermophoretic sampling and transmission electron microscopy, major gas species concentrations by sampling and gas chromatography, concentrations of condensable hydrocarbons by gravimetric sampling. and velocities by laser velocimetry. These data were used to find soot surface growth rates and primary soot particle nucleation rates along the axes of the flames. Present measurements of soot surface growth rates were correlated successfully by predictions based on typical hydrogen-abstraction/carbon-addition (HACA) mechanisms of Frenklach and co-workers and Colket and Hall. These results suavest that reduced soot surface growth rates with increasing residence time seen in the present and other similar flames were mainly caused by reduced rates of surface activation due to reduced H atom concentrations as temperatures decrease as a result of radiative heat losses. Primary soot particle nucleation rates exhibited variations with temperature and acetylene concentrations that were similar to recent observations for diffusion flames; however, nucleation rates in the premixed flames were significantly lower than in, the diffusion flames for reasons that still must be explained. Finally, predictions of yields of major gas species based on mechanisms from both Frenklach and co-workers and Leung and Lindstedt were in good agreement with present measurements and suggest that H atom concentrations (relevant to HACA mechanisms) approximate estimates based on local thermodynamic equilibrium in the present flames.

The use of liquid latex for soot removal from fire scenes and attempted fingerprint development with Ninhydrin.

PubMed

Clutter, Susan Wright; Bailey, Robert; Everly, Jeff C; Mercer, Karl

2009-11-01

Throughout the United States, clearance rates for arson cases remain low due to fire's destructive nature, subsequent suppression, and a misconception by investigators that no forensic evidence remains. Recent research shows that fire scenes can yield fingerprints if soot layers are removed prior to using available fingerprinting processes. An experiment applying liquid latex to sooted surfaces was conducted to assess its potential to remove soot and yield fingerprints after the dried latex was peeled. Latent fingerprints were applied to glass and drywall surfaces, sooted in a controlled burn, and cooled. Liquid latex was sprayed on, dried, and peeled. Results yielded usable prints within the soot prior to removal techniques, but no further fingerprint enhancement was noted with Ninhydrin. Field studies using liquid latex will be continued by the (US) Virginia Fire Marshal Academy but it appears that liquid latex application is a suitable soot removal method for forensic applications.

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

NASA Astrophysics Data System (ADS)

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.

Absorption of visible radiation in atmosphere containing mixtures of absorbing and nonabsorbing particles

NASA Technical Reports Server (NTRS)

Ackerman, T. P.; Toon, O. B.

1981-01-01

The presence of a strongly absorbing material, tentatively identified as graphitic carbon, or 'soot', is indicated by measurements of single-scattering albedo of tropospheric aerosols. Although theoretical calculations based on models of the ways in which soot may mix with other aerosol materials yield the single-scattering albedo values of 0.6, accounted for by a minimum 20% soot by volume, in urban regions and 0.8, yielded by 1-5% soot by volume, in rural settings, it is found that these same values can be produced by similar amounts of the iron oxide magnetite. Magnetite is shown to be indistinguishable from soot by optical measurements performed on bulk samples, and calculation of various mixtures of soot indicate the difficulty of determining aerosol composition by optical scattering techniques.

Effect of alcohol addition on shock-initiated formation of soot from benzene

NASA Technical Reports Server (NTRS)

Frenklach, Michael; Yuan, Tony

1988-01-01

Soot formation in benzene-methanol and benzene-ethanol argon-diluted mixtures was studied behind reflected shock waves by monitoring the attenuation of an He-Ne laser beam. The experiments were performed at temperatures 1580-2250 K, pressures 2.0-3.0 bar, and total carbon atom concentrations (2.0-2.7) x 10 to the 17th atoms/cu cm. The results obtained indicate that the addition of alcohol suppresses the formation of soot from benzene at all temperatures, and that the reduction in soot yields is increased with the amount of alcohol added. The analysis of the results indicates that the suppression effect is probably due to the oxidation of soot and soot precursors by OH and the removal of hydrogen atoms by alcohol and water molecules.

Laser-saturated fluorescence measurements in laminar sooting diffusion flames

NASA Technical Reports Server (NTRS)

Wey, Changlie

1993-01-01

The hydroxyl radical is known to be one of the most important intermediate species in the combustion processes. The hydroxyl radical has also been considered a dominant oxidizer of soot particles in flames. In this investigation the hydroxyl concentration profiles in sooting diffusion flames were measured by the laser-saturated fluorescence (LSF) method. The temperature distributions in the flames were measured by the two-line LSF technique and by thermocouple. In the sooting region the OH fluorescence was too weak to make accurate temperature measurements. The hydroxyl fluorescence profiles for all four flames presented herein show that the OH fluorescence intensities peaked near the flame front. The OH fluorescence intensity dropped sharply toward the dark region of the flame and continued declining to the sooting region. The OH fluorescence profiles also indicate that the OH fluorescence decreased with increasing height in the flames for all flames investigated. Varying the oxidizer composition resulted in a corresponding variation in the maximum OH concentration and the flame temperature. Furthermore, it appears that the maximum OH concentration for each flame increased with increasing flame temperature.

Investigation of the impact of imposed air inlet velocity oscillations on the formation and oxidation of soot using simultaneous 2-Colour-TIRE-LII

NASA Astrophysics Data System (ADS)

Aleksandrov, A.; Suntz, R.; Bockhorn, H.

2015-05-01

The response of non-premixed swirling flames to acoustic perturbations at various frequencies (0-350 Hz) and the impact of imposed air inlet velocity oscillations on the formation and oxidation of soot are investigated. The results obtained from these flames are of special interest for "rich-quenched-lean" (RQL) combustion concepts applied in modern gas turbines. In RQL combustion, the fuel is initially oxidized by air under fuel-rich conditions in a first stage followed by a fuel-lean combustion step in a second stage. To mimic soot formation and oxidation in RQL combustion, soot particle measurements in highly turbulent, non-premixed swirling natural gas/ethylene-confined flames at imposed air inlet velocity oscillations are performed using simultaneous 2-Colour-Time-Resolved-Laser-Induced Incandescence (simultaneous 2-Colour-TIRE-LII). The latter technique is combined with line-of-sight averaged OH*-chemiluminescence imaging, measurements of the velocity field by high-speed particle imaging velocimetry under reactive combustion conditions and measurements of the mean temperature field obtained by a thermocouple. A natural gas/ethylene mixture (Φ = 1.56, 42 % C2H4, 58 % natural gas, P th = 17.6 kW at atmospheric pressure) is used as a fuel, which is oxidized by air under fuel-rich conditions in the first combustion chamber.

Uptake of HNO3 on hexane and aviation kerosene soots.

PubMed

Talukdar, Ranajit K; Loukhovitskaya, Ekaterina E; Popovicheva, Olga B; Ravishankara, A R

2006-08-10

The uptake of HNO(3) on aviation kerosene (TC-1) soot was measured as a function of temperature (253-295 K) and the partial pressure of HNO(3), and the uptake of HNO(3) on hexane soot was studied at 295 K and over a limited partial pressure of HNO(3). The HNO(3) uptake was mostly reversible and did not release measurable amounts of gas-phase products such as HONO, NO(3), NO(2) or N(2)O(5). The heat of adsorption of HNO(3) on soot was dependent on the surface coverage. The isosteric heats of adsorption, Delta(0)H(isosteric), were determined as a function of coverage. Delta(0)H(isosteric) values were in the range -16 to -13 kcal mol(-1). The heats of adsorption decrease with increasing coverage. The adsorption data were fit to Freundlich and to Langmuir-Freundlich isotherms. The heterogeneity parameter values were close to 0.5, which suggested that a HNO(3) molecule can occupy two sites on the surface with or without being dissociated and that the soot surface could be nonuniform. Surface FTIR studies on the interaction of soot with HNO(3) did not reveal formation of any minor product such as organic nitrate or nitro compound on the soot surface. Using our measured coverage, we calculate that the partitioning of gas-phase nitric acid to black carbon aerosol is not a significant loss process of HNO(3) in the atmosphere.

Flow/Soot-Formation Interactions in Nonbuoyant Laminar Diffusion Flames

NASA Technical Reports Server (NTRS)

Dai, Z.; Faeth, G. M.

1999-01-01

Nonpremixed (diffusion) flames are attractive for practical applications because they avoid the stability, autoignition, flashback, etc. problems of premixed flames. Unfortunately, soot formation in practical hydrocarbon-fueled diffusion flames reduces their attractiveness due to widely-recognized public health and combustor durability problems of soot emissions. For example, more deaths are attributed to the emission of soot (15,000-60,000 deaths annually in the U.S. alone) than any other combustion-generated pollutant. In addition, continuum radiation from soot-containing flames is the principle heat load to combustor components and is mainly responsible for engine durability problems of aircraft and gas turbine engines. As a result, there is considerable interest in controlling both soot concentrations within flames and soot emissions from flames. Thus, the objective of the present investigation is to study ways to control soot formation in diffusion flames by manipulating the mixing process between the fuel and oxidant streams. In order to prevent the intrusion of gravity from masking flow properties that reduce soot formation in practical flames (where effects of gravity are small), methods developed during past work will be exploited to minimize effects of buoyant motion.

Reducing Soot in Diesel Exhaust

NASA Technical Reports Server (NTRS)

Bellan, J.

1984-01-01

Electrically charged fuel improves oxidation. Fuel injection system reduces amount of soot formed in diesel engines. Spray injector electrically charges fuel droplets as they enter cylinder. Charged droplets repel each other, creating, dilute fuel mist easily penetrated by oxygen in cylinder.

Large eddy simulation of soot evolution in an aircraft combustor

NASA Astrophysics Data System (ADS)

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-to-air ratio, the maximum soot volume fraction is found inside the recirculation zone; at the lower fuel-to-air ratio, turbulent fluctuations in the mixture fraction promote the oxidation of soot inside the recirculation zone and suppress the accumulation of a large soot volume fraction. Downstream, soot exits the combustor in intermittent fuel-rich pockets that are not mixed during the injection of dilution air and subsequent secondary fuel-lean combustion. At the higher fuel-to-air ratio, the frequency of these fuel-rich pockets is increased, leading to higher soot emissions from the combustor. Quantitatively, the soot emissions from the combustor are overpredicted by about 50%, which is a substantial improvement over previous works utilizing RANS to predict such emissions. In addition, the ratio between the two fuel-to-air ratios predicted by LES compares very favorably with the experimental measurements. Furthermore, soot growth is dominated by an acetylene-based pathway rather than an aromatic-based pathway, which is usually the dominant mechanism in nonpremixed flames. This finding is the result of the interactions between the hydrodynamics, mixing, chemistry, and soot in the recirculation zone and the resulting residence times of soot at various mixture fractions (compositions), which are not the same in this complex recirculating flow as in nonpremixed jet flames.

Temperature, Oxygen, and Soot-Volume-Fraction Measurements in a Turbulent C 2H 4-Fueled Jet Flame

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kearney, Sean P.; Guildenbecher, Daniel Robert; Winters, Caroline

2015-09-01

We present a detailed set of measurements from a piloted, sooting, turbulent C 2 H 4 - fueled diffusion flame. Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (CARS) is used to monitor temperature and oxygen, while laser-induced incandescence (LII) is applied for imaging of the soot volume fraction in the challenging jet-flame environment at Reynolds number, Re = 20,000. Single-laser shot results are used to map the mean and rms statistics, as well as probability densities. LII data from the soot-growth region of the flame are used to benchmark the soot source term for one-dimensional turbulence (ODT) modeling of this turbulentmore » flame. The ODT code is then used to predict temperature and oxygen fluctuations higher in the soot oxidation region higher in the flame.« less

Sub-Scale Analysis of New Large Aircraft Pool Fire-Suppression

DTIC Science & Technology

2016-01-01

discrete ordinates radiation and single step Khan and Greeves soot model provided radiation and soot interaction. Agent spray dynamics were...Notable differences observed showed a modeled increase in the mockup surface heat-up rate as well as a modeled decreased rate of soot production...488 K SUPPRESSION STARTED  Large deviation between sensors due to sensor alignment challenges and asymmetric fuel surface ignition  Unremarkable

Theoretical and Numerical Investigation of Radiative Extinction of Diffusion Flames

NASA Technical Reports Server (NTRS)

Ray, Anjan

1996-01-01

The influence of soot radiation on diffusion flames was investigated using both analytical and numerical techniques. Soot generated in diffusion flames dominate the flame radiation over gaseous combustion products and can significantly lower the temperature of the flame. In low gravity situations there can be significant accumulation of soot and combustion products in the vicinity of the primary reaction zone owing to the absence of any convective buoyant flow. Such situations may result in substantial suppression of chemical activities in a flame, and the possibility of a radiative extinction may also be anticipated. The purpose of this work was to not only investigate the possibility of radiative extinction of a diffusion flame but also to qualitatively and quantitatively analyze the influence of soot radiation on a diffusion flame. In this study, first a hypothetical radiative loss profile of the form of a sech(sup 2) was assumed to influence a pure diffusion flame. It was observed that the reaction zone can, under certain circumstances, move through the radiative loss zone and locate itself on the fuel side of the loss zone contrary to our initial postulate. On increasing the intensity and/or width of the loss zone it was possible to extinguish the flame, and extinction plots were generated. In the presence of a convective flow, however, the movement of the temperature and reaction rate peaks indicated that the flame behavior is more complicated compared to a pure diffusional flame. A comprehensive model of soot formation, oxidation and radiation was used in a more involved analysis. The soot model of Syed, Stewart and Moss was used for soot nucleation and growth and the model of Nagle and Strickland-Constable was used for soot oxidation. The soot radiation was considered in the optically thin limit. An analysis of the flame structure revealed that the radiative loss term is countered both by the reaction term and the diffusion term. The essential balance for the soot volume fraction was found to be between the processes of soot convection and soot growth. Such a balance yielded to analytical treatment and the soot volume fraction could be expressed in the form of an integral. The integral was evaluated using two approximate methods and the results agreed very well with the numerical solutions for all cases examined.

Source apportionment of aerosol particles near a steel plant by electron microscopy.

PubMed

Ebert, Martin; Müller-Ebert, Dörthe; Benker, Nathalie; Weinbruch, Stephan

2012-12-01

The size, morphology and chemical composition of 37,715 individual particles collected over 22 sampling days in the vicinity of a large integrated steel production were studied by scanning and transmission electron microscopy. Based on the morphology, chemistry and beam stability the particles were classified into the following fourteen groups: silicates, sea salt, calcium sulfates, calcium carbonates, carbonate-silicate mixtures, sulfate-silicate mixtures, iron oxides, iron mixtures, metal oxide-metals, complex secondary particles, soot, Cl-rich particles, P-rich particles, and other particles. The majority of iron oxide (≈85%) and metal oxide-metal (≈70%) particles as well as ≈20% of the silicate particles are fly ashes from high temperature processes. The emissions from the steel work are dominated by iron oxide particles. For source apportionment, seven source categories and two sectors of local wind direction (industrial and urban background) were distinguished. In both sectors PM₁₀ consists of four major source categories: 35% secondary, 20% industrial, 17% soil and 16% soot in the urban background sector compared to 45% industrial, 20% secondary, 13% soil, and 9% soot in the industrial sector. As the secondary and the soot components are higher in the urban background sector than in the industrial sector, it is concluded that both components predominantly originate from urban background sources (traffic, coal burning, and domestic heating). Abatement measures should not only focus on the steel work but should also include the urban background aerosol.

Sooting Limits Of Microgravity Spherical Diffusion Flames. [conducted in the NASA Glenn 2.2-second drop tower

NASA Technical Reports Server (NTRS)

Sunderland, P. B.; Urban, D. L.; Stocker, D. P.; Chao, B.-H.; Axelbaum, Richard L.; Salzman, Jack (Technical Monitor)

2001-01-01

Limiting conditions for soot-particle inception were studied in microgravity spherical diffusion flames burning ethylene at atmospheric pressure. Nitrogen was supplied in the fuel and/or oxidizer to obtain the broadest range of stoichiometric mixture fraction. Both normal flames (oxygen in ambience) and inverted flames (fuel in ambience) were considered. Microgravity was obtained in the NASA Glenn 2.2-second drop tower. The flames were observed with a color video camera and sooting conditions were defined as conditions for which yellow emission was present throughout the duration of the drop. Sooting limit results were successfully correlated in terms of adiabatic flame temperature and stoichiometric mixture fraction. Soot free conditions were favored by increased stoichiometric mixture fractions. No statistically significant effect of convection direction on sooting limits was observed. The relationship between adiabatic flame temperature and stoichiometric mixture fraction at the sooting limits was found to be in qualitative agreement with a simple theory based on the assumption that soot inception can occur only where temperature and local C/O ratio exceed threshold values (circa 1250 K and 1, respectively).

Bioaccessibility of PAHs and PAH derivatives in a fuel soot assessed by an in vitro digestive model with absorptive sink: Effects of aging the soot in a soil-water mixture.

PubMed

Zhang, Yanyan; Pignatello, Joseph J; Tao, Shu

2018-02-15

Aging soot in soil under neutral aqueous condition for 30days significantly (p<0.05) reduced the apparent gastrointestinal bioaccessibility (B app ) of polycyclic aromatic hydrocarbons (PAHs) and PAH derivatives (d-PAHs) natively present in a composite fuel soot sample. B app was determined under fasting conditions by a previously developed in vitro digestive model that includes silicone sheet as a third phase absorptive sink in the small intestinal stage. Redistribution of contaminants from soot to soil, determined in independent experiments, was too small to affect B app . Prior uptake by soot of a commercial humic acid representing dissolved soil organic matter had no impact on B app . We identified two causes for the reduction in B app by soil and found they were approximately additive. One is an aging time-independent "matrix effect" attributable to competitive sorption by the soil of labile contaminant that is desorbed from the soot during the digestion test. The other is the dissolution of soluble substances from the soot during the aging process that increases soot surface area and nanoporosity. The increased surface area and nanoporosity drive contaminants from labile to nonlabile states in the soot and decrease the desorption into the digestive fluid, the former contributing most to the reduction in B app . The present study shows that mixing of raw soot with soil has important effects, both aging and non-aging, on the bioaccessibility of soot-borne contaminants. Copyright © 2017 Elsevier B.V. All rights reserved.

Kinetics and mechanism of soot formation in hydrocarbon combustion

NASA Technical Reports Server (NTRS)

Frenklach, Michael

1990-01-01

The focus of this work was on kinetic modeling. The specific objectives were: detailed modeling of soot formation in premixed flames, elucidation of the effects of fuel structure on the pathway to soot, and the development of a numerical technique for accurate modeling of soot particle coagulation and surface growth. Those tasks were successfully completed and are briefly summarized.

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

DTIC Science & Technology

2017-09-09

chemically. Such flames were systematically studied by measuring temperature, species 1. REPORT DATE (DD-MM-YYYY) 4. TITLE AND SUBTITLE 13...pressure) but are still well suited to quantitative diagnostics; 2) Study soot inception by measuring gaseous soot precursors and focusing on the gas-to...downstream across an envelope diffusion flame that is formed between the products of the rich premixed flame and the oxidizer. To mimic this situation, a

Latitudinal distribution of black carbon soot in the upper troposphere and lower stratosphere

NASA Technical Reports Server (NTRS)

Blake, David F.; Kato, Katharine

1995-01-01

Black carbon soot from the upper troposphere and lower stratosphere has been systematically collected at latitudes from 90 deg N to 45 deg S. The measured latitudinal distribution of this soot at 10 to 11 km altitude is found to covary with commercial air traffic fuel use, suggesting that aircraft fuel combustion at altitude is the principal source. In addition, at latitudes where the commercial air traffic is high, measured black carbon soot values are high even at 20 km altitude, suggesting that aircraft-generated soot injected just above the tropopause may be transported to higher altitudes. During the volcanically influenced period in which these samples were collected, the number abundances, total mass, and calculated total surface area of black carbon soot are 2-3 orders of magnitude lower than similar measures of sulfuric acid aerosol. During volcanically quiescent periods, the calculated total surface area of black carbon soot aerosol is of the same order of magnitude as that of the background sulfuric acid aerosol. It appears from this comparison that black carbon soot is only capable of influencing lower stratosphere or upper troposphere chemistry during periods when the aerosol budget is not dominated by volcanic activity. It remains to determine the extent to which black carbon soot particles act as nuclei for sulfuric acid aerosol formation. However, mass balance calculations suggest that aircraft soot injected at altitude does not represent a significant source of condensation nuclei for sulfuric acid aerosols.

Investigation of detailed kinetic scheme performance on modelling of turbulent non-premixed sooting flames

NASA Astrophysics Data System (ADS)

Yunardi, Y.; Darmadi, D.; Hisbullah, H.; Fairweather, M.

2011-12-01

This paper presents the results of an application of a first-order conditional moment closure (CMC) approach coupled with a semi-empirical soot model to investigate the effect of various detailed combustion chemistry schemes on soot formation and destruction in turbulent non-premixed flames. A two-equation soot model representing soot particle nucleation, growth, coagulation and oxidation, was incorporated into the CMC model. The turbulent flow-field of both flames is described using the Favre-averaged fluid-flow equations, applying a standard k-ɛ turbulence model. A number of five reaction kinetic mechanisms having 50-100 species and 200-1000 elementary reactions called ABF, Miller-Bowman, GRI-Mech3.0, Warnatz, and Qin were employed to study the effect of combustion chemistry schemes on soot predictions. The results showed that of various kinetic schemes being studied, each yields similar accuracy in temperature prediction when compared with experimental data. With respect to soot prediction, the kinetic scheme containing benzene elementary reactions tends to result in a better prediction on soot concentrations in comparison to those contain no benzene elementary reactions. Among five kinetic mechanisms being studied, the Qin combustion scheme mechanism turned to yield the best prediction on both flame temperature and soot levels.

Aging fingerprints in combustion particles

NASA Astrophysics Data System (ADS)

Zelenay, V.; Mooser, R.; Tritscher, T.; Křepelová, A.; Heringa, M. F.; Chirico, R.; Prévôt, A. S. H.; Weingartner, E.; Baltensperger, U.; Dommen, J.; Watts, B.; Raabe, J.; Huthwelker, T.; Ammann, M.

2011-05-01

Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing is still a subject of discussion. In this work, soot particles emitted from two different cars, a EURO 2 transporter, a EURO 3 passenger vehicle, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using x-ray absorption spectroscopy and scanning electron microscopy. Comparison of the spectra from the unprocessed and aged soot particles revealed changes in the carbon functional group content, such as that of carboxylic carbon, which can be ascribed to both the condensation of secondary organic compounds on the soot particles and oxidation of primary soot particles upon photochemical aging. Changes in the morphology and size of the single soot particles were also observed upon aging. Furthermore, we show that the soot particles take up water in humid environments and that their water uptake capacity increases with photochemical aging.

Brief Communication: Buoyancy-Induced Differences in Soot Morphology

NASA Technical Reports Server (NTRS)

Ku, Jerry C.; Griffin, Devon W.; Greenberg, Paul S.; Roma, John

1995-01-01

Reduction or elimination of buoyancy in flames affects the dominant mechanisms driving heat transfer, burning rates and flame shape. The absence of buoyancy produces longer residence times for soot formation, clustering and oxidation. In addition, soot pathlines are strongly affected in microgravity. We recently conducted the first experiments comparing soot morphology in normal and reduced-gravity laminar gas jet diffusion flames. Thermophoretic sampling is a relatively new but well-established technique for studying the morphology of soot primaries and aggregates. Although there have been some questions about biasing that may be induced due to sampling, recent analysis by Rosner et al. showed that the sample is not biased when the system under study is operating in the continuum limit. Furthermore, even if the sampling is preferentially biased to larger aggregates, the size-invariant premise of fractal analysis should produce a correct fractal dimension.

Soot formation in shock-tube pyrolysis and oxidation of vinylacetylene

NASA Technical Reports Server (NTRS)

Frenklach, M.; Yuan, T.; Ramachandra, M. K.

1990-01-01

Soot formation in vinylacetylene, and vinylacetylene-oxygen argon-diluted mixtures was studied behind reflected shock waves by monitoring the attenuation of a 632.8-nm He-Ne laser beam. The experiments were performed at temperatures of 1600-2500 K, pressures of 2.08-3.09 bar, and total carbon atom concentrations of (1.99-2.05) x 10 to the 17th atoms/cu cm. The experimental results obtained in pyrolysis of vinylacetylene are similar to those of acetylene, both in the order of magnitude of the soot yield and the shape of its temperature dependence. The addition of oxygen to vinylacetylene shifts the soot bell to lower temperature and, distinct from all other hydrocarbons studied in this laboratory, accelerates the production of soot with reaction time. The experimental results are interpreted in terms of possible chemical reaction.

Nitric Acid Uptake and Decomposition on Black Carbon (Soot) Surfaces: Its Implications for the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Choi, W.; Leu, M. T.

1998-01-01

Black carbon particles (soot) are formed as a result of incomplete combustion processes and are ubiquitous in the atmosphere. The lower troposphere contains plenty of soot particles whose principal sources are fossil fuel and biomass combustion at the ground level.

Shock tube study of the fuel structure effects on the chemical kinetic mechanisms responsible for soot formation, part 2

NASA Technical Reports Server (NTRS)

Frenklach, M.; Clary, D. W.; Ramachandra, M. K.

1985-01-01

Soot formation in oxidation of allene, 1,3-butadiene, vinylacetylene and chlorobenzene and in pyrolysis of ethylene, vinylacetylene, 1-butene, chlorobenzene, acetylen-hydrogen, benzene-acetylene, benzene-butadiene and chlorobenzene-acetylene argon-diluted mixtures was studied behind reflected shock waves. The results are rationalized within the framework of the conceptual models. It is shown that vinylacetylene is much less sooty than allene, which indicates that conjugation by itself is not a sufficient factor for determining the sooting tendency of a molecule. Structural reactivity in the context of the chemical kinetics is the dominant factor in soot formation. Detailed chemical kinetic modeling of soot formation in pyrolysis of acetylene is reported. The main mass growth was found to proceed through a single dominant route composed of conventional radical reactions. The practically irreversible formation reactions of the fused polycyclic aromatics and the overshoot by hydrogen atom over its equilibrium concentration are the g-driving kinetic forces for soot formation.

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

PubMed

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.

Soot and SO2 contribution to the supersites in the MILAGRO campaign from elevated flares in the Tula Refinery

NASA Astrophysics Data System (ADS)

Almanza, V. H.; Molina, L. T.; Sosa, G.

2012-11-01

This work presents a simulation of the plume trajectory emitted by flaring activities of the Miguel Hidalgo Refinery in Mexico. The flame of a representative sour gas flare is modeled with a CFD combustion code in order to estimate emission rates of combustion by-products of interest for air quality: acetylene, ethylene, nitrogen oxides, carbon monoxide, soot and sulfur dioxide. The emission rates of NO2 and SO2 were compared with measurements obtained at Tula as part of MILAGRO field campaign. The rates of soot, VOCs and CO emissions were compared with estimates obtained by Instituto Mexicano del Petróleo (IMP). The emission rates of these species were further included in WRF-Chem model to simulate the chemical transport of the plume from 22 to 27 March of 2006. The model presents reliable performance of the resolved meteorology, with respect to the Mean Absolute Error (MAE), Root Mean Square Error (RMSE), mean bias (BIAS), vector RMSE and Index of Agreement (IOA). WRF-Chem outputs of SO2 and soot were compared with surface measurements obtained at the three supersites of MILAGRO campaign. The results suggest a contribution of Tula flaring activities to the total SO2 levels of 18% to 27% at the urban supersite (T0), and of 10% to 18% at the suburban supersite (T1). For soot, the model predicts low contribution at the three supersites, with less than 0.1% at three supersites. According to the model, the greatest contribution of both pollutants to the three supersites occurred on 23 March, which coincides with the third cold surge event reported during the campaign.

Aeolian Dust and Forest Fire Smoke in Urban Air

NASA Astrophysics Data System (ADS)

Brimblecombe, P.

2006-12-01

Particles of aeolian dust and forest fire smoke are now regularly detected in urban air. Although dusts are common on the Asian Pacific Rim and forest fire smoke characteristic of South East Asia they also frequently detected elsewhere. In the past dust was treated as though it was fairly inert and reactions on the surface limited to the neutralizing ability of alkaline minerals. More recent work shows that that dust has a complex organic chemistry. Observations in China found fatty acids from urban areas (oleic acid and linoleic acid from cooking) on dust derived aerosols. The fatty acids and PAHs decreased sharply after dust storms, suggesting a role for dust in removal processes. When silica particles absorb unsaturated compounds they can react with ozone and release compounds such as formaldehyde. Particles from forest fires have a similarly complex chemistry and the acid-alkaline balance may vary depend on the balance of removal rates of alkaline materials (ammonia, potassium carbonate) and inorganic and organic acids. Airborne dust and forest fire soot can contain humic like substances (HULIS) either as primary material or as secondary oxidation products of the surface of soot. This paper will report on the role polluted air masses in the generation humic materials, particularly those that are surface active. These materials of high molecular weight oxygen rich organic compounds, which exhibit a range of properties of importance in aerosols: they can form complexes with metal ions and thus enhance their solubility, photosensitize the oxidation of organic compounds and lower the surface tension of aqueous aerosols. HULIS can be oxidized to form a range of simpler acids such as formic, acetic and oxalic acid. Dust and forest fire smoke particles have a different composition and size range to that of typical urban combustion particles, so it is likely that the health impacts will be different, yet current regulation often does not recognize any significant difference.

Carbon Nanostructure Examined by Lattice Fringe Analysis of High Resolution Transmission Electron Microscopy Images

NASA Technical Reports Server (NTRS)

VanderWal, Randy L.; Tomasek, Aaron J.; Street, Kenneth; Thompson, William K.

2002-01-01

The dimensions of graphitic layer planes directly affect the reactivity of soot towards oxidation and growth. Quantification of graphitic structure could be used to develop and test correlations between the soot nanostructure and its reactivity. Based upon transmission electron microscopy images, this paper provides a demonstration of the robustness of a fringe image analysis code for determining the level of graphitic structure within nanoscale carbon, i.e. soot. Results, in the form of histograms of graphitic layer plane lengths, are compared to their determination through Raman analysis.

Carbon Nanostructure Examined by Lattice Fringe Analysis of High Resolution Transmission Electron Microscopy Images

NASA Technical Reports Server (NTRS)

VanderWal, Randy L.; Tomasek, Aaron J.; Street, Kenneth; Thompson, William K.; Hull, David R.

2003-01-01

The dimensions of graphitic layer planes directly affect the reactivity of soot towards oxidation and growth. Quantification of graphitic structure could be used to develop and test correlations between the soot nanostructure and its reactivity. Based upon transmission electron microscopy images, this paper provides a demonstration of the robustness of a fringe image analysis code for determining the level of graphitic structure within nanoscale carbon, i.e., soot. Results, in the form of histograms of graphitic layer plane lengths, are compared to their determination through Raman analysis.

Aging induced changes on NEXAFS fingerprints in individual combustion particles

NASA Astrophysics Data System (ADS)

Zelenay, V.; Mooser, R.; Tritscher, T.; Křepelová, A.; Heringa, M. F.; Chirico, R.; Prévôt, A. S. H.; Weingartner, E.; Baltensperger, U.; Dommen, J.; Watts, B.; Raabe, J.; Huthwelker, T.; Ammann, M.

2011-11-01

Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing of the combustion exhaust gases is still a subject of discussion. In this work, individual soot particles emitted from two different vehicles, a EURO 2 transporter, a EURO 3 passenger car, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using near edge X-ray absorption fine structure spectroscopy (NEXAFS) and scanning electron microscopy. Comparison of NEXAFS spectra from the unprocessed particles and those resulting from exhaust photooxidation in the chamber revealed changes in the carbon functional group content. For the wood stove emissions, these changes were minor, related to the relatively mild oxidation conditions. For the EURO 2 transporter emissions, the most apparent change was that of carboxylic carbon from oxidized organic compounds condensing on the primary soot particles. For the EURO 3 car emissions oxidation of primary soot particles upon photochemical aging has likely contributed as well. Overall, the changes in the NEXAFS fingerprints were in qualitative agreement with data from an aerosol mass spectrometer. Furthermore, by taking full advantage of our in situ microreactor concept, we show that the soot particles from all three combustion sources changed their ability to take up water under humid conditions upon photochemical aging of the exhaust. Due to the selectivity and sensitivity of the NEXAFS technique for the water mass, also small amounts of water taken up into the internal voids of agglomerated particles could be detected. Because such small amounts of water uptake do not lead to measurable changes in particle diameter, it may remain beyond the limits of volume growth measurements, especially for larger agglomerated particles.

Trace Metals in Soot and PM2.5 from Heavy-Fuel-Oil Combustion in a Marine Engine

PubMed Central

2018-01-01

Heavy fuel oil (HFO) particulate matter (PM) emitted by marine engines is known to contain toxic heavy metals, including vanadium (V) and nickel (Ni). The toxicity of such metals will depend on the their chemical state, size distribution, and mixing state. Using online soot-particle aerosol mass spectrometry (SP-AMS), we quantified the mass of five metals (V, Ni, Fe, Na, and Ba) in HFO-PM soot particles produced by a marine diesel research engine. The in-soot metal concentrations were compared to in-PM2.5 measurements by inductively coupled plasma-optical emission spectroscopy (ICP-OES). We found that <3% of total PM2.5 metals was associated with soot particles, which may still be sufficient to influence in-cylinder soot burnout rates. Since these metals were most likely present as oxides, whereas studies on lower-temperature boilers report a predominance of sulfates, this result implies that the toxicity of HFO PM depends on its combustion conditions. Finally, we observed a 4-to-25-fold enhancement in the ratio V:Ni in soot particles versus PM2.5, indicating an enrichment of V in soot due to its lower nucleation/condensation temperature. As this enrichment mechanism is not dependent on soot formation, V is expected to be generally enriched within smaller HFO-PM particles from marine engines, enhancing its toxicity. PMID:29688717

Laser Diagnostic Analyses of Sooting Flames.

DTIC Science & Technology

1984-11-29

flame front as expected. However the fuel flame length is considerably shorter than the luminous height, and the flame surface must cross the soot surface...very useful in understanding this behaviour and the fact that the fuel flame length increases only slightly on addition of diluent--while the visible

Electron microscopic study of soot particulate matter emissions from aircraft turbine engines.

PubMed

Liati, Anthi; Brem, Benjamin T; Durdina, Lukas; Vögtli, Melanie; Dasilva, Yadira Arroyo Rojas; Eggenschwiler, Panayotis Dimopoulos; Wang, Jing

2014-09-16

The microscopic characteristics of soot particulate matter (PM) in gas turbine exhaust are critical for an accurate assessment of the potential impacts of the aviation industry on the environment and human health. The morphology and internal structure of soot particles emitted from a CFM 56-7B26/3 turbofan engine were analyzed in an electron microscopic study, down to the nanoscale, for ∼ 100%, ∼ 65%, and ∼ 7% static engine thrust as a proxy for takeoff, cruising, and taxiing, respectively. Sampling was performed directly on transmission electron microscopy (TEM) grids with a state-of-the-art sampling system designed for nonvolatile particulate matter. The electron microscopy results reveal that ∼ 100% thrust produces the highest amount of soot, the highest soot particle volume, and the largest and most crystalline primary soot particles with the lowest oxidative reactivity. The opposite is the case for soot produced during taxiing, where primary soot particles are smallest and most reactive and the soot amount and volume are lowest. The microscopic characteristics of cruising condition soot resemble the ones of the ∼ 100% thrust conditions, but they are more moderate. Real time online measurements of number and mass concentration show also a clear correlation with engine thrust level, comparable with the TEM study. The results of the present work, in particular the small size of primary soot particles present in the exhaust (modes of 24, 20, and 13 nm in diameter for ∼ 100%, ∼ 65% and ∼ 7% engine thrust, respectively) could be a concern for human health and the environment and merit further study. This work further emphasizes the significance of the detailed morphological characteristics of soot for assessing environmental impacts.

Laboratory Studies of Heterogeneous Chemical Processes of Atmospheric Importance

NASA Technical Reports Server (NTRS)

Molina, Mario J.

2004-01-01

The objective of this study is to conduct measurements of chemical kinetics parameters for heterogeneous reactions of importance in the stratosphere and the troposphere. It involves the elucidation of the mechanism of the interaction of HCl vapor with ice surfaces, which is the first step in the heterogeneous chlorine activation processes, as well as the investigation of the atmospheric oxidation mechanism of soot particles emitted by biomass and fossil fuels. The techniques being employed include turbulent flow-chemical ionization mass spectrometry and optical ellipsometry, among others.

Candle Soot-Driven Performance Enhancement in Pyroelectric Energy Conversion

NASA Astrophysics Data System (ADS)

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.

Bulk and surface structural investigations of diesel engine soot and carbon black.

PubMed

Müller, J-O; Su, D S; Wild, U; Schlögl, R

2007-08-14

The microstructure and electronic structure of environmentally relevant carbons such as Euro IV heavy duty diesel engine soot, soot from a black smoking diesel engine, spark discharge soot as model aerosol, commercial furnace soot and lamp black are investigated by transmission electron microscopy, electron energy-loss spectroscopy and X-ray photoelectron spectroscopy. The materials exhibit differences in the predominant bonding, which influences microstructure as well as surface functionalization. These chemical and physical properties depend on the formation history of the investigated carbonaceous materials. In this work, a correlation of the microstructure of the samples to the predominant bonding and incorporation of oxygen into the carbons is obtained. It is shown that a high amount of defects and the deviation of the carbons from a perfect graphitic structure results in a increased incorporation of oxygen and hydrogen. A correlation between the length and curvature of graphene layers with the bonding state of carbon atoms and incorporation of oxygen and hydrogen is established.

Effects of C/O Ratio and Temperature on Sooting Limits of Spherical Diffusion Flames

NASA Technical Reports Server (NTRS)

Lecoustre, V. R.; Sunderland, P. B.; Chao, B. H.; Urban, D. L.; Stocker, D. P.; Axelbaum, R. L.

2008-01-01

Limiting conditions for soot particle inception in spherical diffusion flames were investigated numerically. The flames were modeled using a one-dimensional, time accurate diffusion flame code with detailed chemistry and transport and an optically thick radiation model. Seventeen normal and inverse flames were considered, covering a wide range of stoichiometric mixture fraction, adiabatic flame temperature, residence time and scalar dissipation rate. These flames were previously observed to reach their sooting limits after 2 s of microgravity. Sooting-limit diffusion flames with scalar dissipation rate lower than 2/s were found to have temperatures near 1400 K where C/O = 0.51, whereas flames with greater scalar dissipation rate required increased temperatures. This finding was valid across a broad range of fuel and oxidizer compositions and convection directions.

Soot Imaging and Measurement

NASA Technical Reports Server (NTRS)

1996-01-01

Soot, sometimes referred to as smoke, is made up primarily of the carbon particles generated by most combustion processes. For example, large quantities of soot can be seen issuing from the exhaust pipes of diesel-powered vehicles. Heated soot also is responsible for the warm orange color of candle flames, though that soot is generally consumed before it can exit the flame. Research has suggested that heavy atmospheric soot concentrations aggravate conditions such as pneumonia and asthma, causing many deaths each year. To understand the formation and oxidation of soot, NASA Lewis Research Center scientists, together with several university investigators, are investigating the properties of soot generated in reduced gravity, where the absence of buoyancy allows more time for the particles to grow. The increased time allows researchers to better study the life cycle of these particles, with the hope that increased understanding will lead to better control strategies. To quantify the amount of soot present in a flame, Lewis scientists developed a unique imaging technique that provides quantitative and qualitative soot data over a large field of view. There is significant improvement over the single-point methods normally used. The technique is shown in the sketch, where light from a laser is expanded with a microscope objective, rendered parallel, and passed through a flame where soot particles reduce the amount of light transmitted to the camera. A filter only allows light at the wavelength of the laser to pass to the camera, preventing any extraneous signals. When images of the laser light with and without the flame are compared, a quantitative map of the soot concentration is produced. In addition to that data, a qualitative image of the soot in the flame is also generated, an example of which is displayed in the photo. This technique has the potential to be adapted to real-time process control in industrial powerplants.

Atomic Oxygen Treatment Technique for Removal of Smoke Damage from Paintings

NASA Technical Reports Server (NTRS)

Rutledge, S. K.; Banks, B. A.

1997-01-01

Soot deposits that can accumulate on surfaces of a painting during a fire can be difficult to clean from some types of paintings without damaging the underlying paint layers. A non-contact technique has been developed which can remove the soot by allowing a gas containing atomic oxygen to flow over the surface and chemically react with the soot to form carbon monoxide and carbon dioxide. The reaction is limited to the surface, so the underlying paint is not touched. The process can be controlled so that the cleaning can be stopped once the paint surface is reached. This paper describes the smoke exposure and cleaning of untreated canvas, acrylic gesso, and sections of an oil painting using this technique. The samples were characterized by optical microscopy and reflectance spectroscopy.

Characterization of Air Plane Soot Surrogates using Raman spectroscopy and laser ablation techniques

NASA Astrophysics Data System (ADS)

Chazallon, Bertrand; Ortega, Ismael Kenneth; Ikhenazene, Raouf; Pirim, Claire; Carpentier, Yvain; Irimiea, Cornelia; Focsa, Cristian; Ouf, François-Xavier

2016-04-01

Aviation alters the composition of the atmosphere globally and can thus drive climate change and ozone depletion [1]. Aircraft exhaust plumes contain species (gases and soot particles) produced by the combustion of kerosene with ambient air in the combustion chamber of the engine. Soot particles emitted by air-planes produce persistent contrails in the upper troposphere in ice-supersaturated air masses that contribute to cloudiness and impact the radiative properties of the atmosphere. These aerosol-cloud interactions represent one of the largest sources of uncertainty in global climate models [2]. Though the formation of atmospheric ice particles has been studied for many years [3], there are still numerous opened questions on nucleation properties of soot particles [4], as the ice nucleation experiments showed a large spread in results depending on the nucleation mode chosen and origin of the soot produced. The reasons behind these discrepancies reside in the different physico-chemical properties (composition, structure) of soot particles produced in different conditions, e.g., with respect to fuel or combustion techniques. In this work, we use Raman microscopy (514 and 785 nm excitation wavelengths) and ablation techniques (Secondary Ions Mass Spectrometry, and Laser Desorption Mass Spectrometry) to characterize soot particle surrogates produced from a CAST generator (propane fuel, four different global equivalence ratios). They are produced as analogues of air-plane soot collected at different engine regimes (PowerJet SaM-146 turbofan) simulating a landing and take-off (LTO) cycle (MERMOSE project (http://mermose.onera.fr/)) [6]. The spectral parameters of the first-order Raman bands of these soot samples are analyzed using a de-convolution approach described by Sadezky et al. (2005) [5]. A systematic Raman analysis is carried out to select a number of parameters (laser wavelength, irradiance at sample, exposure time) that will alter the sample and the resulting spectra. If much literature discussed the most appropriate values of these parameters for analyzing graphite, coals, or amorphous carbon, only few works have dealt with soot, and no published studies have proposed the optimal parameter values for air-plane soot surrogates. In this work, we present the effect of three Raman parameters (laser wavelength, irradiance at sample, exposure time) on air-plane soot surrogates. The obtained results qualitatively indicate higher reactivity of soot samples collected in specific air-oxidation conditions. The surface chemical composition of the soot particles with special focus on PAHs are analyzed by two-Step (Desorption/Ionization) Laser Mass Spectrometry (L2MS) and Time of Fight Secondary Ion Mass Spectrometry (ToF-SIMS) techniques. In both techniques the spectra are obtained using positive polarity, which is better suited for detection of PAHs. A good agreement was obtained between the two techniques for the total PAH content of the analyzed samples. CAST samples are further processed by Raman spectroscopy to get complementary information on their structure. References [1] Lee et al., Atmos. Env. 44, 4678-4734, 2010 [2] IPCC 2014, Chap7: http://www.ipcc.ch [3] L. Dufour, Ciel et Terre, vol 82, p1-36, 1966 [4] C. Hoose & O. Möhler, Atmos.Chem.Phys. 12, 9817-9854, 2012 [5] Sadezky, A., Muckenhuber, H., Grothe, H., Niessner, R. and Pöschl U., (2005) Carbon, 43, 1731-1742. [6] Parent, Laffon, Marhaba, Ferry, Regier, Ortega, Chazallon, Carpentier, Focsa, (2016) Carbon (accepted)

Measurements of soot formation and hydroxyl concentration in near critical equivalence ratio premixed ethylene flame

NASA Technical Reports Server (NTRS)

Inbody, Michael Andrew

1993-01-01

The testing and development of existing global and detailed chemical kinetic models for soot formation requires measurements of soot and radical concentrations in flames. A clearer understanding of soot particle inception relies upon the evaluation and refinement of these models in comparison with such measurements. We present measurements of soot formation and hydroxyl (OH) concentration in sequences of flat premixed atmospheric-pressure C2H4/O2/N2 flames and 80-torr C2H4/O2 flames for a unique range of equivalence ratios bracketting the critical equivalence ratio (phi(sub c)) and extending to more heavily sooting conditions. Soot volume fraction and number density profiles are measured using a laser scattering-extinction apparatus capable of resolving a 0.1 percent absorption. Hydroxyl number density profiles are measured using laser-induced fluorescence (LIF) with broadband detection. Temperature profiles are obtained from Rayleigh scattering measurements. The relative volume fraction and number density profiles of the richer sooting flames exhibit the expected trends in soot formation. In near-phi(sub c) visibility sooting flames, particle scattering and extinction are not detected, but an LIF signal due to polycyclic aromatic hydrocarbons (PAH's) can be detected upon excitation with an argon-ion laser. A linear correlation between the argon-ion LIF and the soot volume fraction implies a common mechanistic source for the growth of PAH's and soot particles. The peak OH number density in both the atmospheric and 80-torr flames declines with increasing equivalence ratio, but the profile shape remains unchanged in the transition to sooting, implying that the primary reaction pathways for OH remain unchanged over this transition. Chemical kinetic modeling is demonstrated by comparing predictions using two current reaction mechanisms with the atmospheric flame data. The measured and predicted OH number density profiles show good agreement. The predicted benzene number density profiles correlate with the measured trends in soot formation, although anomalies in the benzene profiles for the richer and cooler sooting flames suggest a need for the inclusion of benzene oxidation reactions.

Assessing the effects of UVA photocatalysis on soot-coated TiO2-containing mortars.

PubMed

De la Rosa, José M; Miller, Ana Z; Pozo-Antonio, J Santiago; González-Pérez, José A; Jiménez-Morillo, Nicasio T; Dionisio, Amelia

2017-12-15

The deposition of soot on building surfaces darkens their colour and leads to undesirable black crusts, which are one of the most serious problems on the conservation of built cultural heritage. As a preventive strategy, self-cleaning systems based on the use of titanium dioxide (TiO 2 ) coatings have been employed on building materials for degrading organic compounds deposited on building surfaces, improving their durability and performance. In this study, the self-cleaning effect of TiO 2 -containing mortars coated with diesel soot has been appraised under laboratory conditions. The mortar samples were manufactured using lime putty and two different doses of TiO 2 (2.5% and 5%). The lime mortars were then coated with diesel engine soot and irradiated with ultraviolet A (UVA) illumination for 30days. The photocatalytic efficiency was evaluated by visual inspection, field emission scanning electron microscopy (FESEM) and colour spectrophotometry. Changes in the chemical composition of the soot particles (including persistent organic pollutants) were assessed by analytical pyrolysis (Py-GC/MS) and solid state 13 C NMR spectroscopy. The FESEM and colour spectrophotometry revealed that the soot-coated TiO 2 -containing mortars promoted a self-cleaning effect after UVA irradiation. The combination of analytical pyrolysis and 13 C solid state NMR showed that the UVA irradiation caused the cracking of polycyclic aromatic structures and n-alkyl compounds of the diesel soot and its transformation into methyl polymers. Our findings also revealed that the inclusion of TiO 2 in the lime mortar formulations catalysed these transformations promoting the self-cleaning of the soot-stained mortars. The combined action of TiO 2 and UVA irradiation is a promising proxy to clean lime mortars affected by soot deposition. Copyright © 2017 Elsevier B.V. All rights reserved.

Cytotoxicity and reactive oxygen species generation from aggregated carbon and carbonaceous nanoparticulate materials

PubMed Central

Garza, Kristine M; Soto, Karla F; Murr, Lawrence E

2008-01-01

We have investigated the cytotoxicity and reactive oxygen species (ROS) generation for indoor and outdoor soots: candle, wood, diesel, tire, and natural gas burner soots – along with surrogate black carbon, various multiwall carbon nanotube aggregate materials, TiO2 (anatase) and chrysotile asbestos as reference materials. All soots were observed utilizing TEM and FESEM to be composed of aggregated, primary spherules (20–80 nm diameter) forming complex, branched fractal structures. These spherules were composed of intercalated, turbostratic arrangements of curved graphene fragments with varying concentrations of polycyclic aromatic hydrocarbon (PAH) isomers. In vitro cultures with an immortalized human lung epithelial carcinoma cell line (A549) treated with these materials showed decreased cell viability and variations in ROS production, with no correlations to PAH content. The data demonstrate that soots are cytotoxic and that cytotoxicity is not related to PAH content but is related to ROS generation, suggesting that soot induces cellular oxidative stress and that cell viability assays can be indicators of ROS production. PMID:18488419

Optical and Probe Diagnostics Applied to Reacting Flows

NASA Technical Reports Server (NTRS)

Ticich, Thomas M.

2003-01-01

The general theme of the research my NASA colleague and I have planned is "Optical and probe diagnostics applied to reacting flows". We plan to explore three major threads during the fellowship period. The first interrogates the flame synthesis of carbon nanotubes using aerosol catalysts. Having demonstrated the viability of the technique for nanotube synthesis, we seek to understand the details of this reacting system which are important to its practical application. Laser light scattering will reveal changes in particle size at various heights above the burner. Analysis of the flame gas by mass spectroscopy will reveal the chemical composition of the mixture. Finally, absorption measurements will map the nanotube concentration within the flow. The second thread explores soot oxidation kinetics. Despite the impact of soot on engine performance, fire safety and pollution, models for its oxidation are inhibited by uncertainty in the values of the oxidation rate. We plan to employ both optical and microscopic measurements to refine this rate. Cavity ring-down absorption measurements of the carbonaceous aerosol can provide a measure of the mass concentration with time and, hence, an oxidation rate. Spectroscopic and direct probe measurements will provide the temperature of the system needed for subsequent modeling. These data will be benchmarked against changes in soot nanostructures as revealed by transmission electron microscopic images from directly sampled material.

Combustion characteristics of the LO2/GCH4 fuel-rich preburners for staged combustion cycle rocket engines

NASA Astrophysics Data System (ADS)

Ono, Fumiei; Tamura, Hiroshi; Sakamoto, Hiroshi; Sasaki, Masaki

1991-09-01

The combustion characteristics of Liquid Oxygen (LO2)/Gaseous Methane (GCH4) fuel rich preburners were experimentally studied using subscale hardware. Three types of preburners with coaxial type propellant injection elements were designed and fabricated, and were used for hot fire testing. LO2 was used as oxidizer, and GCH4 at room temperature was used as fuel. The tests were conducted at chamber pressures ranging from 6.7 to 11.9 M Pa, and oxidizer to fuel ratios ranged from 0.16 to 0.42. The test results, which include combustion gas temperature T(sub c), characteristic velocity C(sup *) and soot adhesion data, are presented. The T(sub c) efficiency and the C(sup *) efficiency were found to be a function of oxidizer to fuel ratio and chamber pressure. These efficiencies are correlated by an empirical correlation parameter which accounts for the effects of oxidizer to fuel ratio and chamber pressure. The exhaust plumes were colorless and transparent under all tests conditions. There was some soot adhesion to the chamber wall, but no soot adhesion was observed on the main injector simulator orifices. Higher temperature igniter gas was required to ignite the main propellants of the preburner compared with that of the LO2/Gaseous Hydrogen (GH2) propellants combination.

Validation of an LES Model for Soot Evolution against DNS Data in Turbulent Jet Flames

NASA Astrophysics Data System (ADS)

Mueller, Michael

2012-11-01

An integrated modeling approach for soot evolution in turbulent reacting flows is validated against three-dimensional Direct Numerical Simulation (DNS) data in a set of n-heptane nonpremixed temporal jet flames. As in the DNS study, the evolution of the soot population is described statistically with the Hybrid Method of Moments (HMOM). The oxidation of the fuel and formation of soot precursors are described with the Radiation Flamelet/Progress Variable (RFPV) model that includes an additional transport equation for Polycyclic Aromatic Hydrocarbons (PAH) to account for the slow chemistry governing these species. In addition, the small-scale interactions between soot, chemistry, and turbulence are described with a presumed subfilter PDF approach that accounts for the very large spatial intermittency characterizing soot in turbulent reacting flows. The DNS dataset includes flames at three different Damköhler numbers to study the influence of global mixing rates on the evolution of PAH and soot. In this work, the ability of the model to capture these trends quantitatively as Damköhler number varies is investigated. In order to reliably assess the LES approach, the LES is initialized from the filtered DNS data after an initial transitional period in an effort to minimize the hydrodynamic differences between the DNS and the LES.

Studying the Use of Photocatalytic Coatings to Increase Building/Structure Sustainability and Cleanliness at NASA Stennis Space Center

NASA Technical Reports Server (NTRS)

Underwood, Lauren

2013-01-01

TiO2 coated surfaces demonstrated both visually through photographic representation, and quantitatively, through reflectance measurements that they improved upon the current state of cleanliness upon the surfaces that they were applied to. TiO2 has the potential to both maintain and increase building s sustainability and the overall appearance of cleanliness TiO2 coated slides degraded soot under UV light compared to soot samples on plain uncoated slides under the same conditions Degradation of soot by photocatalysis was far more apparent than degradation of soot by UV light alone This demonstration provides the foundation for a laboratory model that could be used to simulate real world applications for photocatalytic materials Additional research is required to better understand the full potential of TiO2

The rapid alveolar absorption of diesel soot-adsorbed benzo[a]pyrene: bioavailability, metabolism and dosimetry of an inhaled particle-borne carcinogen.

PubMed

Gerde, P; Muggenburg, B A; Lundborg, M; Dahl, A R

2001-05-01

Exposure to diesel exhaust may contribute to lung cancer in humans. It remains unclear whether the carbonaceous core of the soot particle or its coat of adsorbed/condensed organics contributes most to cancer risk. Equally unclear are the extent and rate at which organic procarcinogens desorb from soot particles in the lungs following inhalation exposure and the extent of their metabolic activation in the lungs. To explore the basic relationship between a model polycyclic aromatic hydrocarbon (PAH) and a typical carrier particle, we investigated the rate and extent of release and metabolic fate of benzo[a]pyrene (BaP) adsorbed on the carbonaceous core of diesel soot. The native organic content of the soot had been denuded by toluene extraction. Exogenous BaP was adsorbed onto the denuded soot as a surface coating corresponding to 25% of a monomolecular layer. Dogs were exposed by inhalation to an aerosol bolus of the soot-adsorbed BAP: Following deposition in the alveolar region a fraction of BaP was rapidly desorbed from the soot and quickly absorbed into the circulation. Release rates then decreased drastically. When coatings reached approximately 16% of a monolayer the remaining BaP was not bioavailable and was retained on the particles after 5.6 months in the lung. However, the bioavailability of particles transported to the lymph nodes was markedly higher; after 5.6 months the surface coating of BaP was reduced to 10%. BaP that remained adsorbed on the soot surface after this period was approximately 30% parent compound. In contrast, the rapidly released pulse of BaP, which was quickly absorbed through the alveolar epithelium after inhalation, appeared mostly unmetabolized in the circulation, along with low concentrations of phase I and phase II BaP metabolites. However, within approximately 1 h this rapidly absorbed fraction of BaP was systemically metabolized into mostly conjugated phase II metabolites. The results indicate that absorption through the alveolar epithelium is an important route of entry to the circulation of unmetabolized PAHS:

Rational strategy for the atmospheric icing prevention based on chemically functionalized carbon soot coatings

NASA Astrophysics Data System (ADS)

Esmeryan, Karekin D.; Bressler, Ashton H.; Castano, Carlos E.; Fergusson, Christian P.; Mohammadi, Reza

2016-12-01

Although the superhydrophobic surfaces are preferable for passive anti-icing systems, as they provide water shedding before initiation of ice nucleation, their practical usage is still under debate. This is so, as the superhydrophobic materials are not necessarily icephobic and most of the synthesis techniques are characterized with low fabrication scalability. Here, we describe a rational strategy for the atmospheric icing prevention, based on chemically functionalized carbon soot, suitable for large-scale fabrication of superhydrophobic coatings that exhibit and retain icephobicity in harsh operational conditions. This is achieved through a secondary treatment with ethanol and aqueous fluorocarbon solution, which improves the coating's mechanical strength without altering its water repellency. Subsequent experimental analyses on the impact dynamics of icy water droplets on soot coated aluminum and steel sheets show that these surfaces remain icephobic in condensate environments and substrate temperatures down to -35 °C. Furthermore, the soot's icephobicity and non-wettability are retained in multiple icing/de-icing cycles and upon compressed air scavenging, spinning and water jetting with impact velocity of ∼25 m/s. Finally, on frosted soot surfaces, the droplets freeze in a spherical shape and are entirely detached by adding small amount of thermal energy, indicating lower ice adhesion compared to the uncoated metal substrates.

Explosive decomposition of ethylene oxide at elevated condition: effect of ignition energy, nitrogen dilution, and turbulence.

PubMed

Pekalski, A A; Zevenbergen, J F; Braithwaite, M; Lemkowitz, S M; Pasman, H J

2005-02-14

Experimental and theoretical investigation of explosive decomposition of ethylene oxide (EO) at fixed initial experimental parameters (T=100 degrees C, P=4 bar) in a 20-l sphere was conducted. Safety-related parameters, namely the maximum explosion pressure, the maximum rate of pressure rise, and the Kd values, were experimentally determined for pure ethylene oxide and ethylene oxide diluted with nitrogen. The influence of the ignition energy on the explosion parameters was also studied. All these dependencies are quantified in empirical formulas. Additionally, the effect of turbulence on explosive decomposition of ethylene oxide was investigated. In contrast to previous studies, it is found that turbulence significantly influences the explosion severity parameters, mostly the rate of pressure rise. Thermodynamic models are used to calculate the maximum explosion pressure of pure and of nitrogen-diluted ethylene oxide, at different initial temperatures. Soot formation was experimentally observed. Relation between the amounts of soot formed and the explosion pressure was experimentally observed and was calculated.

Aggregation Kinetics of Diesel Soot Nanoparticles in Wet Environments.

PubMed

Chen, Chengyu; Huang, Weilin

2017-02-21

Soot produced during incomplete combustion consists mainly of carbonaceous nanoparticles (NPs) with severe adverse environmental and health effects, and its environmental fate and transport are largely controlled by aggregation. In this study, we examined the aggregation behavior for diesel soot NPs under aqueous condition in an effort to elucidate the fundamental processes that govern soot particle-particle interactions in wet environments such as rain droplets or surface aquatic systems. The influence of electrolytes and aqueous pH on colloidal stability of these NPs was investigated by measuring their aggregation kinetics in different aqueous solution chemistries. The results showed that the NPs had negatively charged surfaces and exhibited both reaction- and diffusion-limited aggregation regimes with rates depended upon solution chemistry. The aggregation kinetics data were in good agreement with the classic Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The critical coagulation concentrations (CCC) were quantified and the Hamaker constant was derived for the soot (1.4 × 10 -20 J) using the colloidal chemistry approach. The study indicated that, depending upon local aqueous chemistry, single soot NPs could remain stable against self-aggregation in typical freshwater environments and in neutral cloud droplets but are likely to aggregate under salty (e.g., estuaries) or acidic (e.g., acid rain droplets) aquatic conditions or both.

Arctic tundra shrub invasion and soot deposition: Consequences for spring snowmelt and near-surface air temperatures

NASA Astrophysics Data System (ADS)

Strack, John E.

Invasive shrubs and soot pollution both have the potential to alter the surface energy balance and timing of snow melt in the Arctic. Shrubs reduce the amount of snow lost to sublimation on the tundra during the winter leading to a deeper end-of-winter snowpack. The shrubs also enhance the absorption of energy by the snowpack during the melt season, by converting incoming solar radiation to longwave radiation and sensible heat. This results in a faster rate of snow melt, warmer near-surface air temperatures, and a deeper boundary layer. Soot deposition lowers the albedo of the snow allowing it to more effectively absorb incoming solar radiation and thus melt faster. This study uses the Colorado State University Regional Atmospheric Modeling System version 4.4 (CSU-RAMS 4.4), equipped with an enhanced snow model, to investigate the effects of shrub encroachment and soot deposition on the atmosphere and snowpack in the Kuparuk Basin of Alaska during the May-June melt period. The results of the simulations suggest that a complete invasion of the tundra by shrubs leads to a 1.5 degree C warming of 2-m air temperatures, 17 watts per meter square increase in surface sensible heat flux, and a 108 m increase in boundary layer depth during the melt period. The snow free-date also occurred 11 days earlier despite having a larger initial snowpack. The results also show that a decrease in the snow albedo of 0.1, due to soot pollution, caused the snow-free date to occur five days earlier. The soot pollution caused a 0.5 degree C warming of 2-m air temperatures and a 2 watts per meter square increase in surface sensible heat flux. In addition, the boundary layer averaged 25 m deeper in the polluted snow simulation.

Modeling of Fuel Film Cooling on Chamber Hot Wall

DTIC Science & Technology

2014-07-01

downstream, when the film has been depleted of its cooling and coking capacities, a second slot is needed to inject fresh cool fuel. All of these...pyrolysis and oxidation. 7. As discussed in the introductory section, sooting and coking are notoriously complex topics. Well- validated global...accurate models for soot formation and deposition. Instead, the potential impact of the coke layer is evaluated parametrically by representing the

Tribological Behavior of Nano-Onions in Krytox 143AB Evaluated

NASA Technical Reports Server (NTRS)

Street, Kenneth W.; VanderWal, Randy L.; Marchetti, Mario; Tomasek, Aaron J.

2005-01-01

Nanoparticles have been developed over the past 10 years and have found several applications. This work presents the use of carbon nano-onions as a potential oil additive for aerospace applications. Researchers at the NASA Glenn Research Center tested lubricant lifetimes in ambient air and ultrahigh vacuum and characterized the breakdown products of the friction and wear. These carbon nanoparticles can provide adequate lubrication very similar to that of graphitic material when run in air. Soot represents one of the very first nanostructured materials, although it has rarely been considered as such. Changes in the carbon nanostructure, resulting in increased graphitic layer plane length, correlate with reactivity loss. Upon heating spherically shaped nanometer-sized carbon black in the absence of oxidant, graphene sheets form, and the initial soot particle templates the growth of a graphitic particle into what is best described as a sphere with many flat sides having a hollow interior. Because there are no edge sites, these polygonal graphitic particles, or nano-onions, are relatively resistant to oxidation. Graphite is used as a solid lubricant because of its stability at moderately high temperatures. However, the temperature at which graphite oxidizes rapidly is strongly influenced by surface area. With the size of particles typically employed in lubrication, a great amount of thermal stability is lost because of size reduction either during preparation or during lubrication of contacting parts. Therefore, we have undertaken a study of the lubricating ability of graphitic nano-onions (ref. 1).

Heterogeneous nucleation of ice on carbon surfaces.

PubMed

Lupi, Laura; Hudait, Arpa; Molinero, Valeria

2014-02-26

Atmospheric aerosols can promote the heterogeneous nucleation of ice, impacting the radiative properties of clouds and Earth's climate. The experimental investigation of heterogeneous freezing of water droplets by carbonaceous particles reveals widespread ice freezing temperatures. It is not known which structural and chemical characteristics of soot account for the variability in ice nucleation efficiency. Here we use molecular dynamics simulations to investigate the nucleation of ice from liquid water in contact with graphitic surfaces. We find that atomically flat carbon surfaces promote heterogeneous nucleation of ice, while molecularly rough surfaces with the same hydrophobicity do not. Graphitic surfaces and other surfaces that promote ice nucleation induce layering in the interfacial water, suggesting that the order imposed by the surface on liquid water may play an important role in the heterogeneous nucleation mechanism. We investigate a large set of graphitic surfaces of various dimensions and radii of curvature and find that variations in nanostructures alone could account for the spread in the freezing temperatures of ice on soot in experiments. We conclude that a characterization of the nanostructure of soot is needed to predict its ice nucleation efficiency.

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

PubMed

Bardeen, Charles G; Garcia, Rolando R; Toon, Owen B; Conley, Andrew J

2017-09-05

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.

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

NASA Astrophysics Data System (ADS)

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

2017-09-01

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.

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

PubMed Central

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

The Ice Nucleation Activity of Surface Modified Soot

NASA Astrophysics Data System (ADS)

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. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, Wiley-Interscience, N. J., 1998. Zolles, T., Burkart, J., Hausler, T., Pummer, B., Hitzenberger, R., and Grothe, H.: Identification of Ice Nucleation Active Sites on Feldspar Dust Particles, Journal of Physical Chemistry A, 119, 2692-2700, 2015.

Polynuclear aromatic hydrocarbon and particulate emissions from two-stage combustion of polystyrene: the effects of the secondary furnace (afterburner) temperature and soot filtration.

PubMed

Wang, Jun; Richter, Henning; Howard, Jack B; Levendis, Yiannis A; Carlson, Joel

2002-02-15

Laboratory experiments were conducted in a two-stage horizontal muffle furnace in order to monitor emissions from batch combustion of polystyrene (PS) and identify conditions that minimize them. PS is a dominant component of municipal and hospital waste streams. Bench-scale combustion of small samples (0.5 g) of shredded styrofoam cups was conducted in air, using an electrically heated horizontal muffle furnace, kept at Tgas = 1000 degrees C. Upon devolatilization, combustion of the polymer took place in a diffusion flame over the sample. The gaseous combustion products were mixed with additional air in a venturi and were channeled to a secondary muffle furnace (afterburner) kept at Tgas = 900-1100 degrees C; residence time therein varied between 0.6 and 0.8 s. At the exits of the primary and the secondary furnace the emissions of CO, CO2, O2, NOx, particulates as well as volatile and semivolatile hydrocarbons, such as polycyclic aromatic hydrocarbons (PAH), were monitored. Online analyzers, gravimetric techniques, and gas chromatography coupled to mass spectrometry (GC-MS) were used. Experiments were also conducted with a high-temperature barrier filter, placed just before the exit of the primary furnace to prevent the particulates from entering into the secondary furnace. Results demonstrated the beneficial effect of the afterburner in reducing PAH concentrations, including those of mutagenic species such as benzo[a]pyrene. Concentrations of individual PAH exhibited a pronounced after burner temperature dependence, typically ranging from a small decrease at 900 degrees C to a larger degree of consumption at 1100 degrees C. Consumption of PAH was observed to be the dominant feature at 900 degrees C, while significant quantities of benzene and some of its derivatives, captured by means of carbosieve/Carbotrap adsorbents, were formed in the afterburner at a temperature of 1000 degrees C. In the primary furnace, about 30% of the mass of the initial polystyrene was converted into soot, while the total mass of PAH represented about 3% of the initial mass of combustible. The afterburner reduced the particulate (soot) emissions by only 20-30%, which indicates that once soot is formed its destruction is rather difficult because its oxidation kinetics are slow undertypical furnace conditions. Moreover, increasing the afterburnertemperature resulted in an increasing trend of soot emissions therefrom, which might indicate competition between soot oxidation and formation, with some additional formation occurring at the higher temperatures. Contrary to the limited effect of the afterburner, high-temperature filtration of the combustion effluent prior to the exit of the primary furnace allowed for effective soot oxidation inside of the ceramic filter. Filtration drastically reduced soot emissions, by more than 90%. Limited soot formation in the afterburner was again observed with increasing temperatures. The yields of both CO and CO2 were largely unaffected by the temperature of the afterburner but increased at the presence of the filter indicating oxidation therein. A previously developed kinetic model was used to identify major chemical reaction pathways involving PAH in the afterburner. The experimental data at the exit of the primary furnace was used as input to these model computations. A first evaluation of the predictive capability of the model was conducted for the case with ceramic filter and a temperature of 900 degrees C. The afterburner was approximated as a plug-flow reactor, and model predictions at a residence time of 0.8 s were compared to experimental data collected at its exit. In agreement with the experimental PAH concentration, only a minor impact of the afterburner treatment was observed for most species at 900 degrees C. OH was deduced to be the major reactant with a mole fraction about 4 orders of magnitudes higher than that of hydrogen radicals. Evidence for the need of further work on the quantitative assessment of oxidation of PAH and their radicals is given.

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

NASA Technical Reports Server (NTRS)

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 in Laminar Premixed Methane/Oxygen Flames at Atmospheric Pressure. Appendix H

NASA Technical Reports Server (NTRS)

Xu, F.; Lin, K.-C.; Faeth, G. M.; Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2001-01-01

Flame structure and soot formation were studied within soot-containing laminar premixed methanefoxygen 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 hydrogenabstraction/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.

Structure and Soot Formation Properties of Laminar Flames

NASA Technical Reports Server (NTRS)

El-Leathy, A. M.; Xu, F.; Faeth, G. M.

2001-01-01

Soot formation within hydrocarbon-fueled flames is an important unresolved problem of combustion science for several reasons: soot emissions are responsible for more deaths than any other combustion-generated pollutant, thermal loads due to continuum radiation from soot limit the durability of combustors, thermal radiation from soot is mainly responsible for the growth and spread of unwanted fires, carbon monoxide emissions associated with soot emissions are responsible for most fire deaths, and limited understanding of soot processes in flames is a major impediment to the development of computational combustion. Motivated by these observations, soot processes within laminar premixed and nonpremixed (diffusion) flames are being studied during this investigation. The study is limited to laminar flames due to their experimental and computational tractability, noting the relevance of these results to practical flames through laminar flamelet concepts. Nonbuoyant flames are emphasized because buoyancy affects soot processes in laminar diffusion flames whereas effects of buoyancy are small for most practical flames. This study involves both ground- and space-based experiments, however, the following discussion will be limited to ground-based experiments because no space-based experiments were carried out during the report period. The objective of this work was to complete measurements in both premixed and nonpremixed flames in order to gain a better understanding of the structure of the soot-containing region and processes of soot nucleation and surface growth in these environments, with the latter information to be used to develop reliable ways of predicting soot properties in practical flames. The present discussion is brief, more details about the portions of the investigation considered here can be found in refs. 8-13.

Using Carbon-14 Isotope Tracing to Investigate Molecular Structure Effects of the Oxygenate Dibutyl Maleate on Soot Emissions from a DI Diesel Engine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buchholz, B A; Mueller, C J; Upatnieks, A

2004-01-07

The effect of oxygenate molecular structure on soot emissions from a DI diesel engine was examined using carbon-14 ({sup 14}C) isotope tracing. Carbon atoms in three distinct chemical structures within the diesel oxygenate dibutyl maleate (DBM) were labeled with {sup 14}C. The {sup 14}C from the labeled DBM was then detected in engine-out particulate matter (PM), in-cylinder deposits, and CO{sub 2} emissions using accelerator mass spectrometry (AMS). The results indicate that molecular structure plays an important role in determining whether a specific carbon atom either does or does not form soot. Chemical-kinetic modeling results indicate that structures that produce CO{submore » 2} directly from the fuel are less effective at reducing soot than structures that produce CO before producing CO{sub 2}. Because they can follow individual carbon atoms through a real combustion process, {sup 14}C isotope tracing studies help strengthen the connection between actual engine emissions and chemical-kinetic models of combustion and soot formation/oxidation processes.« less

A New Paradigm in Modeling and Simulations of Complex Oxidation Chemistry Using a Statistical Approach

DTIC Science & Technology

2009-03-31

8. This range encompasses diesel , HCCI and gas turbine engines , including cold ignition; and NOx , CO and soot pollutant formation in the lean and...equivalence ratios from 0.125 to 8. This range encompasses diesel , HCCI and gas turbine engines , including cold ignition; and NOx , CO and soot pollutant...California Institute of Technology Mechanical Engineering Department Pasadena CA 91125 i Abstract This report describes a study

Oxidation kinetics and soot formation

NASA Technical Reports Server (NTRS)

Glassman, I.; Brezinsky, K.

1983-01-01

The research objective is to clarify the role of aromaticity in the soot nucleation process by determining the relative importance of phenyl radical/molecular oxygen and benzene/atomic oxygen reactions in the complex combustion of aromatic compounds. Three sets of chemical flow reactor experiments have been designed to determine the relative importance of the phenyl radical/molecular oxygen and benzene/atomic oxygen reactions. The essential elements of these experiments are 1) the use of cresols and anisole formed during the high temperature oxidation of toluene as chemical reaction indicators; 2) the in situ photolysis of molecular oxygen to provide an oxygen atom perturbation in the reacting aromatic system; and 3) the high temperature pyrolysis of phenol, the cresols and possibly anisole.

Influence and efficiency of catalytic stripper in organic carbon removal from laboratory generated soot aerosols

EPA Science Inventory

A catalytic stripper (CS) is a device used to remove the semi-volatile, typically organic carbon, fraction by passing raw or diluted exhaust over an oxidation catalyst heated to 300˚C. The oxidation catalyst used in this study is a commercially available diesel oxidation ca...

Soot Aerosol Properties in Laminar Soot-Emitting Microgravity Nonpremixed Flames

NASA Technical Reports Server (NTRS)

Konsur, Bogdan; Megaridis, Constantine M.; Griffin, Devon W.

1999-01-01

The spatial distributions and morphological properties of the soot aerosol are examined experimentally in a series of 0-g laminar gas-jet nonpremixed flames. The methodology deploys round jet diffusion flames of nitrogen-diluted acetylene fuel burning in quiescent air at atmospheric pressure. Full-field laser-light extinction is utilized to determine transient soot spatial distributions within the flames. Thermophoretic sampling is employed in conjunction with transmission electron microscopy to define soot microstructure within the soot-emitting 0-g flames. The microgravity tests indicate that the 0-g flames attain a quasi-steady state roughly 0.7 s after ignition, and sustain their annular structure even beyond their luminous flame tip. The measured peak soot volume fractions show a complex dependence on burner exit conditions, and decrease in a nonlinear fashion with decreasing characteristic flow residence times. Fuel preheat by approximately 140 K appears to accelerate the formation of soot near the flame axis via enhanced fuel pyrolysis rates. The increased soot presence caused by the elevated fuel injection temperatures triggers higher flame radiative losses, which may account for the premature suppression of soot growth observed along the annular region of preheated-fuel flames. Electron micrographs of soot aggregates collected in 0-g reveal the presence of soot precursor particles near the symmetry axis at midflame height, The observations also verify that soot primary particle sizes are nearly uniform among aggregates present at the same flame location, but vary considerably with radius at a fixed distance from the burner. The maximum primary size in 0-g is found to be by 40% larger than in 1-g, under the same burner exit conditions. Estimates of the number concentration of primary particles and surface area of soot particulate phase per unit volume of the combustion gases are also made for selected in-flame locations.

Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties

DOE PAGES

China, Swarup; Scarnato, Barbara; Owen, Robert C.; ...

2015-01-14

The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. In this paper, we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of ≤2.17. The top of the atmosphere directmore » radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. Lastly, the forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.« less

Interdigitated Pt-GaN Schottky interfaces for high-temperature soot-particulate sensing

NASA Astrophysics Data System (ADS)

So, Hongyun; Hou, Minmin; Jain, Sambhav R.; Lim, Jongwoo; Senesky, Debbie G.

2016-04-01

A microscale soot-particulate sensor using interdigitated platinum-gallium nitride (Pt-GaN) Schottky interfaces was developed to monitor fine soot particles within high-temperature environments (e.g., combustion exhausts and flues). Upon exposure to soot particles (30 to 50 nm in diameter) from an experimental chimney, an increased current (∼43.6%) is observed through the back-to-back Schottky contact to n-type GaN. This is attributed to a reduction in the effective Schottky barrier height (SBH) of ∼10 meV due to the electric field from the charged soot particles in the depletion region and exposed GaN surface. Furthermore, the microfabricated sensor was shown to recover sensitivity and regenerate the sensing response (∼11 meV SBH reduction) after exposure to temperature as high as 550 °C. This study supports the feasibility of a simple and reliable soot sensor to meet the increasing market demand for particulate matter sensing in harsh environments.

Microwave-Based Oxidation State and Soot Loading Determination on Gasoline Particulate Filters with Three-Way Catalyst Coating for Homogenously Operated Gasoline Engines.

PubMed

Dietrich, Markus; Jahn, Christoph; Lanzerath, Peter; Moos, Ralf

2015-09-02

Recently, a novel method emerged to determine the oxygen storage degree of three way catalysts (TWC) by a microwave-based method. Up to now, this method has been investigated only in lab-scale reactors or under steady state conditions. This work expands those initial studies. A TWC-coated gasoline particulate filter was investigated in a dynamic engine test bench simulating a typical European driving cycle (NEDC). It could be shown that both the oxygen storage degree and the soot loading can be monitored directly, but not simultaneously due to their competitive effects. Under normal driving conditions, no soot accumulation was observed, related to the low raw emissions and the catalytic coating of the filter. For the first time, the quality factor of the cavity resonator in addition to the resonance frequency was used, with the benefit of less cross sensitivity to inconstant temperature and water. Therefore, a temperature dependent calibration of the microwave signal was created and applied to monitor the oxidation state in transient driving cycles. The microwave measurement mirrors the oxidation state determined by lambda probes and can be highly beneficial in start-stop phases (where lambda-probes do not work) and to determine the oxygen storage capacity (OSC) without unnecessary emissions.

Microwave-Based Oxidation State and Soot Loading Determination on Gasoline Particulate Filters with Three-Way Catalyst Coating for Homogenously Operated Gasoline Engines

PubMed Central

Dietrich, Markus; Jahn, Christoph; Lanzerath, Peter; Moos, Ralf

2015-01-01

Recently, a novel method emerged to determine the oxygen storage degree of three way catalysts (TWC) by a microwave-based method. Up to now, this method has been investigated only in lab-scale reactors or under steady state conditions. This work expands those initial studies. A TWC-coated gasoline particulate filter was investigated in a dynamic engine test bench simulating a typical European driving cycle (NEDC). It could be shown that both the oxygen storage degree and the soot loading can be monitored directly, but not simultaneously due to their competitive effects. Under normal driving conditions, no soot accumulation was observed, related to the low raw emissions and the catalytic coating of the filter. For the first time, the quality factor of the cavity resonator in addition to the resonance frequency was used, with the benefit of less cross sensitivity to inconstant temperature and water. Therefore, a temperature dependent calibration of the microwave signal was created and applied to monitor the oxidation state in transient driving cycles. The microwave measurement mirrors the oxidation state determined by lambda probes and can be highly beneficial in start-stop phases (where lambda-probes do not work) and to determine the oxygen storage capacity (OSC) without unnecessary emissions. PMID:26340629

An FT-IR study of the effect of simulated solar radiation and various particulates on the oxidation of SO/sub 2/

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, D. M.; Keifer, J. R.; Novicky, M.

1989-01-01

Short- and long-term studies of the effect of black carbon and otherparticulates on the oxidation of SO/sub 2/, with an without the presence ofoxygen, water vapor, and simulated solar radiation, have been carriedout. FT-IR studies involving isotopic oxygen-18, sulfur dioxide-18, and D/sub 2/Oin these reactions confirm the requirement of water vapor and oxygen forthis oxidation. Such experiments conducted at 298 K demonstrate only theformation of ionic sulfates, while the reactions conducted under simulatedsolar radiation show the formation of both covalent and ionic sulfate species.These observations have implications for the retention or diminution ofcatalytic activity by the soot. The reaction vesselmore » walls, SiO/sub 2/, andparticulate black carbon, all act as catalysts for the conversion ofS(IV) to S(VI), the amounts depending primarily on the surface area of thesolid.« less

Ordered micro/macro porous K-OMS-2/SiO2 nanocatalysts: Facile synthesis, low cost and high catalytic activity for diesel soot combustion

PubMed Central

Yu, Xuehua; Zhao, Zhen; Wei, Yuechang; Liu, Jian

2017-01-01

A series of novel oxide catalysts, which contain three-dimensionally ordered macroporous (3DOM) and microporous structure, were firstly designed and successfully synthesized by simple method. In the as-prepared catalysts, 3DOM SiO2 is used as support and microporous K-OMS-2 oxide nanoparticles are supported on the wall of SiO2. 3DOM K-OMS-2/SiO2 oxide catalysts were firstly used in soot particle oxidation reaction and they show very high catalytic activities. The high activities of K-OMS-2/SiO2 oxide catalysts can be assigned to three possible reasons: macroporous effect of 3DOM structure for improving contact between soot and catalyst, microporous effect of K-OMS-2 for adsorption of small gas molecules and interaction of K and Mn for activation of gas molecules. The catalytic activities of catalysts are comparable to or even higher than noble metal catalyst in the medium and high temperature range. For example, the T50 of K-OMS-2/SiO2-50, 328 °C, is much lower than those of Pt/Al2O3 and 3DOM Au/LaFeO3, 464 and 356 °C,respectively. Moreover, catalysts exhibited high catalytic stability. It is attributed to that the K+ ions are introduced into the microporous structure of OMS-2 and stabilized in the catalytic reaction. Meanwhile, the K+ ions play an important role in templating and stabilizing the tunneled framework of OMS-2. PMID:28443610

Wall temperature measurements at elevated pressures and high temperatures in sooting flames in a gas turbine model combustor

NASA Astrophysics Data System (ADS)

Nau, Patrick; Yin, Zhiyao; Geigle, Klaus Peter; Meier, Wolfgang

2017-12-01

Wall temperatures were measured with thermographic phosphors on the quartz walls of a model combustor in ethylene/air swirl flames at 3 bar. Three operating conditions were investigated with different stoichiometries and with or without additional injection of oxidation air downstream of the primary combustion zone. YAG:Eu and YAG:Dy were used to cover a total temperature range of 1000-1800 K. Measurements were challenging due to the high thermal background from soot and window degradation at high temperatures. The heat flux through the windows was estimated from the temperature gradient between the in- and outside of the windows. Differences in temperature and heat flux density profiles for the investigated cases can be explained very well with the previously measured differences in flame temperatures and flame shapes. The heat loss relative to thermal load is quite similar for all investigated flames (15-16%). The results complement previous measurements in these flames to investigate soot formation and oxidation. It is expected, that the data set is a valuable input for numerical simulations of these flames.

Fuel-rich catalytic combustion: A soot-free technique for in situ hydrogen-like enrichment

NASA Technical Reports Server (NTRS)

Brabbs, T. A.; Olson, S. L.

1985-01-01

An experimental program on the catalytic oxidation of iso-octane demonstrated the feasibility of the two-stage combustion system for reducing particulate emissions. With a fuel-rich (phi = 4.8 to 7.8) catalytic combustion preburner as the first stage the combustion process was soot free at reactor outlet temperatures of 1200 K or less. Although soot was not measured directly, its absence was indicated. Reaction products collected at two positions downstream of the catalyst bed were analyzed on a gas chromatograph. Comparison of these products indicated that pyrolysis of the larger molecules continued along the drift tube and that benzene formation was a gas-phase reaction. The effective hydrogen-carbon ratio calculated from the reaction products increased by 20 to 68 percent over the range of equivalence ratios tested. The catalytic partial oxidation process also yielded a large number of smaller-containing molecules. The fraction of fuel carbon in compounds having two or fewer carbon atoms ranged from 30 percent at 1100 K to 80 percent at 1200 K.

Atomic layer deposition of cerium oxide for potential use in diesel soot combustion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ivanova, Tatiana V., E-mail: tatiana.ivanova@lut.fi, E-mail: ivanova.tatyana.v@gmail.com; Toivonen, Jenni; Maydannik, Philipp S.

The particulate soot emission from diesel motors has a severe impact on the environment and people's health. The use of catalytic convertors is one of the ways to minimize the emission and decrease the hazard level. In this paper, the activity of cerium oxide for catalytic combustion of diesel soot was studied. Thin films of cerium dioxide were synthesized by atomic layer deposition using tetrakis(2,2,6,6-tetramethyl-3,5-heptanedionato)cerium [Ce(thd){sub 4}] and ozone as precursors. The characteristics of the films were studied as a function of deposition conditions within the reaction temperature range of 180–350 °C. Thickness, crystallinity, elemental composition, and morphology of the CeO{submore » 2} films deposited on Si (100) were characterized by ellipsometry, x-ray diffraction, x-ray photoelectron spectroscopy, atomic force microscopy, and field emission scanning electron microscopy, respectively. The growth rate of CeO{sub 2} was observed to be 0.30 Å/cycle at temperatures up to 250 °C with a slight increase to 0.37 Å/cycle at 300 °C. The effect of CeO{sub 2} films grown on stainless steel foil supports on soot combustion was measured with annealing tests. Based on the analysis of these, in catalytic applications, CeO{sub 2} has been shown to be effective in lowering the soot combustion temperature from 600 °C for the uncoated substrates to 370 °C for the CeO{sub 2} coated ones. It was found that the higher deposition temperatures had a positive effect on the catalyst performance.« less

Atomic Oxygen Treatment as a Method of Recovering Smoke Damaged Paintings

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Banks, Bruce A.; Forkapa, Mark; Stueber, Thomas; Sechkar, Edward; Malinowski, Kevin

1998-01-01

Smoke damage, as a result of a fire, can be difficult to remove from some types of painting media without causing swelling, leaching or pigment movement or removal. A non-contact technique has been developed which can remove soot from the surface of a painting by use of a gently flowing gas containing atomic oxygen. The atomic oxygen chemically reacts with the soot on the surface creating gasses such as carbon monoxide and carbon dioxide which can be removed through the use of an exhaust system. The reaction is limited to the surface so that the process can be timed to stop when the paint layer is reached. Atomic oxygen is a primary component of the low Earth orbital environment, but can be generated on Earth through various methods. This paper will discuss the results of atomic oxygen treatment of soot exposed acrylic gesso, ink on paper, and a varnished oil painting. Reflectance measurements were used to characterize the surfaces before and after treatment.

Mixing weight determination for retrieving optical properties of polluted dust with MODIS and AERONET data

NASA Astrophysics Data System (ADS)

Chang, Kuo-En; Hsiao, Ta-Chih; Hsu, N. Christina; Lin, Neng-Huei; Wang, Sheng-Hsiang; Liu, Gin-Rong; Liu, Chian-Yi; Lin, Tang-Huang

2016-08-01

In this study, an approach in determining effective mixing weight of soot aggregates from dust-soot aerosols is proposed to improve the accuracy of retrieving properties of polluted dusts by means of satellite remote sensing. Based on a pre-computed database containing several variables (such as wavelength, refractive index, soot mixing weight, surface reflectivity, observation geometries and aerosol optical depth (AOD)), the fan-shaped look-up tables can be drawn out accordingly for determining the mixing weights, AOD and single scattering albedo (SSA) of polluted dusts simultaneously with auxiliary regional dust properties and surface reflectivity. To validate the performance of the approach in this study, 6 cases study of polluted dusts (dust-soot aerosols) in Lower Egypt and Israel were examined with the ground-based measurements through AErosol RObotic NETwork (AERONET). The results show that the mean absolute differences could be reduced from 32.95% to 6.56% in AOD and from 2.67% to 0.83% in SSA retrievals for MODIS aerosol products when referenced to AERONET measurements, demonstrating the soundness of the proposed approach under different levels of dust loading, mixing weight and surface reflectivity. Furthermore, the developed algorithm is capable of providing the spatial distribution of the mixing weights and removing the requirement to assume that the dust plume properties are uniform. The case study further shows the spatially variant dust-soot mixing weight would improve the retrieval accuracy in AODmixture and SSAmixture about 10.0% and 1.4% respectively.

Synthesis of carbon nanotubes by arc discharge in open air.

PubMed

Paladugu, Mohan Chand; Maneesh, K; Nair, P Kesavan; Haridoss, Prathap

2005-05-01

In this work Carbon nanotubes have been synthesized by arc discharge in open air. A TIG welding ac/dc inverter was used as the power source for arc discharge. During each run of the arc discharge based synthesis, the anode was a low purity (approximately 85% C by weight) graphite rod. The effect of varying the atmosphere on the yield of soot of the carbon nanotube containing carbon soot has been studied. Various soots were produced, purified by oxidation and characterized to confirm formation of carbon nanotubes and their relative quality, using transmission electron microscopy, Raman spectroscopy, and XRD. It was found that the yield of soot formed on the cathode is higher when synthesis is carried out in open air than when carried out in a flowing argon atmosphere. When synthesized in open air, using a 7.2-mm-diameter graphite rod as anode, the yield of soot was around 50% by weight of the graphite consumed. Current and voltage for arcing were at identical starting values in all the experiments. This modified method does not require a controlled atmosphere as in the case of a conventional arc discharge method of synthesis and hence the cost of production may be reduced.

Gunshot residue patterns on skin in angled contact and near contact gunshot wounds.

PubMed

Plattner, T; Kneubuehl, B; Thali, M; Zollinger, U

2003-12-17

The goal of this study was the reproduction of shape and pattern of gunshot residues in near contact and contact gunshot wounds by a series of experimental gunshots on a skin and soft tissue model. The aim was to investigate the shape and direction of soot deposits with regard to the muzzle according to different muzzle-target angles, firing distances, type of ammunition and weapon and barrel length. Based on a review of the literature and on the results of the experiments the authors could make the following statements of gunshot residues in angled contact and close contact gunshot: (1) gunshot residues on the target surface can be differentiated in a "inner" and "outer powder soot zone"; (2) the outer powder soot zone is much less visible than the inner powder soot zone and may lack on human skin; (3) with increasing muzzle target distance both inner and outer powder soot halo increase in size and decrease in density; (4) in angled shots the inner powder soot halo shows an eccentric, elliptic shape which points towards the muzzle, regardless of ammunition, calibre and barrel length; (5) the outer powder soot points away from the muzzle in angled contact and close contact shots.

Combustion of droplets and sprays

NASA Astrophysics Data System (ADS)

Eigenbrod, Christian; Sattelmayer, Thomas; Bäßler, Stefan; Mauss, Fabian; Meisl, Jürgen; Oomens, Bas; Rackwitz, Leif; Tait, Nigel; Angelberger, Christian; Eilts, Peter; Magnusson, Ingemar; Lauvergne, Romain; Tatschl, Reinhard

2005-10-01

The combustion of liquid hydrocarbon fuels in internal combustion engines and gas turbines for energy production and aircraft propulsion is intrinsically tied to the formation of pollutants. Apart from aiming for the highest combustion efficiencies in order to lower the operational costs and the emission of CO2, the reduction of poisonous and environmentally harmful exhaust constituents is a challenging task for scientists and engineers. The most prominent pollutants are soot, identified to trigger respiratory diseases and cancer, and nitric oxides such as NO and NO2, which promote the formation of ozone affecting the cardiovascular system when released in the lower atmosphere. Soot and nitric oxides are greenhouse pollutants in the upper atmosphere. Even though only 2-3% of the anthropogenic emission of nitric oxides are contributed by aircraft, it is the only emission at high altitudes. Unfortunately, it has the greatest impact on climate there and it does not matter whether the fuels are fossil or, in the future, biomass.

Investigation of a tripropylene-glycol monomethyl ether and diesel blend for soot-free combustion in an optical direct-injection diesel engine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dumitrescu, Cosmin E.; Mueller, Charles J.; Kurtz, Eric

Natural luminosity and chemiluminescence imaging diagnostics were employed to investigate if a 50/50 blend by volume of tripropylene-glycol monomethyl ether (TPGME) and ultra-low sulfur #2 diesel certification fuel (CF) could enable leaner-lifted flame combustion (LLFC), a non-sooting mode of mixing-controlled combustion associated with equivalence ratios below approximately 2. The experiments were performed in a singlecylinder heavy-duty optical compression-ignition engine at three injection pressures and three dilution levels. Results indicate that TPGME addition effectively eliminated engine-out smoke emissions by curtailing soot production and/or increasing soot oxidation during and after the end of fuel injection. TPGME greatly reduced soot luminosity when compared with neat CF, but did not enable LLFC because the equivalence ratios at the lift-off length,more » $$\\phi$$(H), never reached the non-sooting limit. Nevertheless, this study showed that TPGME addition has the potential to enable LLFC under different experimental conditions that would further decrease $$\\phi$$(H) to ~ 2 and below. Concerning other engine-out emissions, injection pressure influenced the effects of TPGME addition on NO x emissions. Finally, HC and CO emissions were higher compared to baseline fuel likely due to the lower net heat of combustion of TPGME and the need to limit fuel-injection duration for valid optical measurements.« less

Investigation of a tripropylene-glycol monomethyl ether and diesel blend for soot-free combustion in an optical direct-injection diesel engine

DOE PAGES

Dumitrescu, Cosmin E.; Mueller, Charles J.; Kurtz, Eric

2015-12-31

Natural luminosity and chemiluminescence imaging diagnostics were employed to investigate if a 50/50 blend by volume of tripropylene-glycol monomethyl ether (TPGME) and ultra-low sulfur #2 diesel certification fuel (CF) could enable leaner-lifted flame combustion (LLFC), a non-sooting mode of mixing-controlled combustion associated with equivalence ratios below approximately 2. The experiments were performed in a singlecylinder heavy-duty optical compression-ignition engine at three injection pressures and three dilution levels. Results indicate that TPGME addition effectively eliminated engine-out smoke emissions by curtailing soot production and/or increasing soot oxidation during and after the end of fuel injection. TPGME greatly reduced soot luminosity when compared with neat CF, but did not enable LLFC because the equivalence ratios at the lift-off length,more » $$\\phi$$(H), never reached the non-sooting limit. Nevertheless, this study showed that TPGME addition has the potential to enable LLFC under different experimental conditions that would further decrease $$\\phi$$(H) to ~ 2 and below. Concerning other engine-out emissions, injection pressure influenced the effects of TPGME addition on NO x emissions. Finally, HC and CO emissions were higher compared to baseline fuel likely due to the lower net heat of combustion of TPGME and the need to limit fuel-injection duration for valid optical measurements.« less

Combustion products of 1,3-butadiene are cytotoxic and genotoxic to human bronchial epithelial cells.

PubMed Central

Catallo, W J; Kennedy, C H; Henk, W; Barker, S A; Grace, S C; Penn, A

2001-01-01

Adverse health effects of airborne toxicants, especially small respirable particles and their associated adsorbed chemicals, are of growing concern to health professionals, governmental agencies, and the general public. Areas rich in petrochemical processing facilities (e.g., eastern Texas and southern California) chronically have poor air quality. Atmospheric releases of products of incomplete combustion (e.g., soot) from these facilities are not subject to rigorous regulatory enforcement. Although soot can include respirable particles and carcinogens, the toxicologic and epidemiologic consequences of exposure to environmentally relevant complex soots have not been well investigated. Here we continue our physico-chemical analysis of butadiene soot and report effects of exposure to this soot on putative targets, normal human bronchial epithelial (NHBE) cells. We examined organic extracts of butadiene soot by gas chromatography-mass spectrometry (GC-MS), probe distillation MS, and liquid chromatography (LC)-MS-MS. Hundreds of aromatic hydrocarbons and polycyclic aromatic hydrocarbons with molecular mass as high as 1,000 atomic mass units were detected, including known and suspected human carcinogens (e.g., benzo(a)pyrene). Butadiene soot particles also had strong, solid-state free-radical character in electron spin resonance analysis. Spin-trapping studies indicated that fresh butadiene soot in a buffered aqueous solution containing dimethylsulfoxide (DMSO) oxidized the DMSO, leading to CH(3)* radical formation. Butadiene soot DMSO extract (BSDE)-exposed NHBE cells displayed extranuclear fluorescence within 4 hr of exposure. BSDE was cytotoxic to > 20% of the cells at 72 hr. Morphologic alterations, including cell swelling and membrane blebbing, were apparent within 24 hr of exposure. These alterations are characteristic of oncosis, an ischemia-induced form of cell death. BSDE treatment also produced significant genotoxicity, as indicated by binucleated cell formation. The combination of moderate cytotoxicity and genotoxicity, as occurred here, can be pro-carcinogenic. PMID:11673128

Improved adhesion of ultra-hard carbon films on cobalt–chromium orthopaedic implant alloy

PubMed Central

Vaid, Rishi; Diggins, Patrick; Weimer, Jeffrey J.; Koopman, M.; Vohra, Yogesh K.

2010-01-01

While interfacial graphite formation and subsequent poor film adhesion is commonly reported for chemical vapor deposited hard carbon films on cobalt-based materials, we find the presence of O2 in the feedgas mixture to be useful in achieving adhesion on a CoCrMo alloy. Nucleation studies of surface structure before formation of fully coalesced hard carbon films reveal that O2 feedgas helps mask the catalytic effect of cobalt with carbon through early formation of chromium oxides and carbides. The chromium oxides, in particular, act as a diffusion barrier to cobalt, minimizing its migration to the surface where it would otherwise interact deleteriously with carbon to form graphite. When O2 is not used, graphitic soot forms and films delaminate readily upon cooling to room temperature. Continuous 1 μm-thick nanostructured carbon films grown with O2 remain adhered with measured hardness of 60 GPa and show stable, non-catastrophic circumferential micro-cracks near the edges of indent craters made using Rockwell indentation. PMID:21221739

Enhanced photoluminescence and characterization of multicolor carbon dots using plant soot as a carbon source.

PubMed

Tan, Mingqian; Zhang, Lingxin; Tang, Rong; Song, Xiaojie; Li, Yimin; Wu, Hao; Wang, Yanfang; Lv, Guojun; Liu, Wanfa; Ma, Xiaojun

2013-10-15

Carbon dots (C-dots) are a class of novel fluorescent nanomaterials, which have drawn great attention for their potential applications in bio-nanotechnology. Multicolor C-dots have been synthesized by chemical nitric acid oxidation using the reproducible plant soot as raw material. TEM analysis reveals that the prepared C-dots have an average size of 3.1 nm. The C-dots are well dispersed in aqueous solution and are strongly fluorescent under the irradiation of ultra-violet light. X-ray photoelectron spectroscopy characterization demonstrates that the O/C atomic ratio for C-dots change to from 0.207 to 0.436 due to the chemical oxidation process. The photo bleaching experiment reveals that the C-dots show excellent photostability as compared with the conventional organic dyes, fluorescein and rhodamine B. The fluorescence intensity of the C-dots did not change significantly in the pH range of 3-10. To further enhance the fluorescence quantum yield, the C-dots were surface modified with four types of passivation ligands, 4,7,10-trioxa-1,13-tridecanediamine (TTDDA), poly-L-lysine (PLL), cysteine and chitosan and the fluorescence quantum yields of the TTDDA, PLL, cysteine and chitosan passivated C-dots were improved 1.53-, 5.94-, 2.00- and 3.68-fold, respectively. Fourier-transform infrared (FTIR) spectra were employed to characterize the surface groups of the C-dots. The bio-application of the C-dots as fluorescent bio-probes was evaluated in cell imaging and ex vivo fish imaging, which suggests that the C-dots may have potential applications in biolabeling and bioimaging. Copyright © 2013 Elsevier B.V. All rights reserved.

Fuel Efficient Diesel Particulate Filter (DPF) Modeling and Development

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stewart, Mark L.; Gallant, Thomas R.; Kim, Do Heui

The project described in this report seeks to promote effective diesel particulate filter technology with minimum fuel penalty by enhancing fundamental understanding of filtration mechanisms through targeted experiments and computer simulations. The overall backpressure of a filtration system depends upon complex interactions of particulate matter and ash with the microscopic pores in filter media. Better characterization of these phenomena is essential for exhaust system optimization. The acicular mullite (ACM) diesel particulate filter substrate is under continuing development by Dow Automotive. ACM is made up of long mullite crystals which intersect to form filter wall framework and protrude from the wallmore » surface into the DPF channels. ACM filters have been demonstrated to effectively remove diesel exhaust particles while maintaining relatively low backpressure. Modeling approaches developed for more conventional ceramic filter materials, such as silicon carbide and cordierite, have been difficult to apply to ACM because of properties arising from its unique microstructure. Penetration of soot into the high-porosity region of projecting crystal structures leads to a somewhat extended depth filtration mode, but with less dramatic increases in pressure drop than are normally observed during depth filtration in cordierite or silicon carbide filters. Another consequence is greater contact between the soot and solid surfaces, which may enhance the action of some catalyst coatings in filter regeneration. The projecting crystals appear to provide a two-fold benefit for maintaining low backpressures during filter loading: they help prevent soot from being forced into the throats of pores in the lower porosity region of the filter wall, and they also tend to support the forming filter cake, resulting in lower average cake density and higher permeability. Other simulations suggest that soot deposits may also tend to form at the tips of projecting crystals due to the axial velocity component of exhaust moving down the filter inlet channel. Soot mass collected in this way would have a smaller impact on backpressure than soot forced into the flow restrictions deeper in the porous wall structure. This project has focused on the development of computational, analytical, and experimental techniques that are generally applicable to a wide variety of exhaust aftertreatment technologies. By helping to develop improved fundamental understanding pore-scale phenomena affecting filtration, soot oxidation, and NOX abatement, this cooperative research and development agreement (CRADA) has also assisted Dow Automotive in continuing development and commercialization of the ACM filter substrate. Over the course of this research project, ACM filters were successfully deployed on the Audi R10 TDI racecar which won the 24 Hours of LeMans endurance race in 2006, 2007, and 2008; and the 12 Hours of Sebring endurance race in 2006 and 2007. It would not have been possible for the R10 to compete in these traditionally gasoline-dominated events without reliable and effective exhaust particulate filtration. These successes demonstrated not only the performance of automotive diesel engines, but the efficacy of DPF technology as it was being deployed around the world to meet new emissions standards on consumer vehicles. During the course of this CRADA project, Dow Automotive commercialized their ACM DPF technology under the AERIFYTM DPF brand.« less

Arctic tundra shrub invasion and soot deposition: Consequences for spring snowmelt and near-surface air temperatures

NASA Astrophysics Data System (ADS)

Strack, John E.; Pielke, Roger A.; Liston, Glen E.

2007-12-01

Invasive shrubs and soot pollution both have the potential to alter the surface energy balance and timing of snow melt in the Arctic. Shrubs reduce the amount of snow lost to sublimation on the tundra during the winter leading to a deeper end-of-winter snowpack. The shrubs also enhance the absorption of energy by the snowpack during the melt season by converting incoming solar radiation to longwave radiation and sensible heat. Soot deposition lowers the albedo of the snow, allowing it to more effectively absorb incoming solar radiation and thus melt faster. This study uses the Colorado State University Regional Atmospheric Modeling System version 4.4 (CSU-RAMS 4.4), equipped with an enhanced snow model, to investigate the effects of shrub encroachment and soot deposition on the atmosphere and snowpack in the Kuparuk Basin of Alaska during the May-June melt period. The results of the simulations suggest that a complete invasion of the tundra by shrubs leads to a 2.2°C warming of 3 m air temperatures and a 108 m increase in boundary layer depth during the melt period. The snow-free date also occurred 11 d earlier despite having a larger initial snowpack. The results also show that a decrease in the snow albedo of 0.1, owing to soot pollution, caused the snow-free date to occur 5 d earlier. The soot pollution caused a 1.0°C warming of 3 m air temperatures and a 25 m average deepening of the boundary layer.

Climate Effects and Efficacy of Dust and Soot in Snow

NASA Astrophysics Data System (ADS)

Zender, C. S.; Flanner, M. G.; Randerson, J. T.; Mahowald, N. M.; Rasch, P. J.; Yoshioka, M.; Painter, T.

2006-12-01

Dust and industrial and biomass burning emissions from low and mid-latitudes dominate the absorbing impurities trapped in snow at mid- and high-latitudes. We study the effects of dust and smoke on global and regional climate using a general circulation model driven by observed and predicted aerosol emissions determined from satellite and in situ observations. The model has sophisticated treatments of aerosol and snowpack radiative and thermodynamic processes that compare well with observations of snow albedo evolution and impurity concentration. This presentation focuses on the individual and combined contributions of present day dust and soot to snow-albedo forcing and on the global temperature and snowpack responses. Results are emphasized near India and East Asia, where the anthropogenic aerosol forcing of surface albedo and hydrology is greatest. We find that dust and black carbon (BC) aerosols have climate change efficacies (surface temperature change per unit forcing) about 3--4 times greater than CO2, making them the most efficacious forcing agents known. We estimate present day dust and soot snowpack-forcing of ~ 0.050 W m-2 warms global climate by ~ 0.16 °K. Anthropogenic soot from fossil fuel sources causes more than 50% of this warming, and biomass burning can account for up to 30% in strong tropical or boreal burn years. The greatest forcings occur in the Tarim/Mongol region (due to dust), northeastern China (due to soot), and the Tibetan Plateau (both). Dirty springtime snow in these regions can darken albedo by more than 0.1 and increase surface absorption by more than 20 W m-2. These results have implications for the strength of the Asian Monsoon, which is negatively correlated with antecedent snow cover in non-ENSO years. Dust and soot have such strong efficacies because they increase spring melt rates thus reduce summer snow cover. In some regions and seasons, dirty snow reduces snowpack depth and cover by 50%, triggering strong snow and sea-ice albedo feedbacks.

Experimental Study of Unsupported Nonane fuel Droplet Combustion in Microgravity

NASA Technical Reports Server (NTRS)

Callahan, B. J.; Avedisian, C. T.; Hertzog, D. E.; Berkery, J. W.

1999-01-01

Soot formation in droplet flames is the basic component of the particulate emission process that occurs in spray combustion. The complexity of soot formation motivates a one-dimensional transport condition which has obvious advantages in modeling. Recent models of spherically symmetric droplet combustion have made this assumption when incorporating such aspects as detailed chemistry and radiation. Interestingly, spherical symmetry does not necessarily restrict the results because it has been observed that the properties of carbon formed in flames are not strongly affected by the nature of the fuel or flaming configuration. What is affected, however, are the forces acting on the soot aggregates and where they are trapped by a balance of drag and thermophoretic forces. The distribution of these forces depends on the transport conditions of the flame. Prior studies of spherical droplet flames have examined the droplet burning history of alkanes, alcohols and aromatics. Data are typically the evolution of droplet, flame, extinction, and soot shell diameters. These data are only now just beginning to find their way into comprehensive numerical models of droplet combustion to test proposed oxidation schemes for fuels such as methanol and heptane. In the present study, we report new measurements on the burning history of unsupported nonane droplets in a convection-free environment to promote spherical symmetry. The far-field gas is atmospheric pressure air at room temperature. The evolution of droplet diameter was measured using high speed cine photography of a spark-ignited, droplet within a confined volume in a drop tower. The initial droplet diameters varied between 0.5 mm and 0.6 mm. The challenge of unsupported droplets is to form, deploy and ignite them with minimal disturbance, and then to keep them in the camera field of view. Because of the difficulty of this undertaking, more sophisticated diagnostics for studying soot than photographic were not used. Supporting the test droplet by a fiber fixes the droplet position but the fiber can perturb the burning process especially for a sooting fuel. Prior studies on heptane showed little evidence for soot formation due to g-droplets of similar size the relationship between sooting and droplet diameter. For nonane droplets we expect increased sooting due to the greater number of carbon atoms. As a sooting droplet burns and its diameter decreases, proportionally less soot should form. This reduced soot, as well as the influence of soot formed earlier in the burning process which collects in a 'shell', on heat transport to the flame offers the potential for a time-varying burning rate. Such an effect was investigated and revealed in results reported here. Speculation is offered for the cause of this effect and its possible relation to soot formation.

Evolution of Soot Particle Morphology and Mixing State in the Atmosphere

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; China, S.; Sharma, N.; Gorkowski, K.; Dubey, M.; Aiken, A. C.; Zaveri, R. A.; Salvadori, N.; Chakrabarty, R. K.; Moosmuller, H.; Onasch, T. B.; Herndon, S.; Williams, L. R.; Liu, S.; Dzepina, K.; Helmig, D.; Hueber, J.; Fialho, P. J.; Mazzoleni, L. R.; kumar, S.; Dziobak, M.; Wright, K.

2013-12-01

Soot particles (aka black carbon) impact the environment and climate by affecting Earth's radiation balance, cloud microphysics, and atmospheric chemistry. The complex morphology and mixing state of soot particles influence their optical properties and therefore their radiative forcing, the particles' transport, lifecycle, and heterogeneous chemistry. How soot morphology and mixing state alter during transport from the source to remote areas is still not well understood. While aging, soot particles can change shape, oxidize and mix, and become coated by organic and inorganic materials. In this study, we investigate the morphological and mixing state evolution of single soot particles in different stages of their 'life' in the atmosphere. This analysis will include an overview of several samples collected in various locations and atmospheric conditions: 1) particles freshly emitted near freeway on-ramps in Southern Michigan (USA); 2) particles emitted in two biomass burning events in New Mexico (USA), one close to the sampling location and another hundreds of miles away; 3) particles in the urban atmosphere of Mexico City and in the uplifted boundary layer captured on the top of the Pico de Tres Padres Mountain (on the north edge of Mexico City); 4) particles collected in the Sacramento urban area and the Sierra Nevada foothills (CA, USA); 5) particles collected in Detling (UK), and mostly transported from London, and 6) long-range transported particles in the free troposphere and collected at the Pico Mountain Observatory, located near the top of the Pico Volcano in the Azores (Portugal). We analyzed a large number of individual particles using electron microscopy and X-ray spectroscopy followed by image analysis. The projected structural properties of soot particles were characterized using size (maximum length, maximum width, and area equivalent diameter) and shape descriptors (e.g., aspect ratio, roundness, and convexity). The particle mass-fractal dimensions were determined using the ensemble method. The mixing state was analyzed by classifying soot particles based on visual inspection of coating and morphology. Soot particles freshly emitted by anthropogenic sources show less coating and more open chain-like structures; on the other hand biomass burning and long-range transported soot particles appear to be mostly coated and exhibit very compacted shapes. However, soot processing in urban atmospheres results in a complex mixture of coated and uncoated particles with a variety of morphologies and mixing states.

Superhydrophobicity of hierarchical nanostructure of candle soot films

NASA Astrophysics Data System (ADS)

Hankhuntond, A.; Singjai, P.; Sakulsermsuk, S.

2017-09-01

Candle soot containing carbon nanoparticles can form hierarchical structure films. We prepared soot films by using glass slides blocking candle flame in the middle of the flame. The hierarchical nanostructures of the carbon nanoparticles films were confirmed by scanning electron microscopy and transmission electron microscopy. Carbon nanoparticle size was 49.2 ± 9.0 nm from SEM, which agrees to 37.9 ± 8.5 nm from TEM. The contact angles of water droplets on these films are more than 150°, indicating superhydrophobic surface. Decrease contact angles of water droplets were observed with an increase deposition time. The decrease of contact angle was saturated at about 150° when the deposition time reaches 180 s. Cassie-Baxter state was attributed to describe superhydrophobicity of carbon nanoparticles films because the hierarchical nanostructures of the surface provide a large fraction of hollows on the surface. We proposed that the contact angle dependence on deposition time was governed by the increase of the distance between nanopillars in carbon nanoparticles films.

Computational Investigation of Soot and Radiation in Turbulent Reacting Flows

NASA Astrophysics Data System (ADS)

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 scalars from the LES are used in conjunction with the radiation heat transfer equation and a narrow band radiation model to compute time dependent and time averaged images of infrared radiation intensity in spectral bands corresponding to molecular radiation from gas phase carbon dioxide and soot particles exclusively. While qualitative and quantitative comparisons with measured images in the CO2 radiation band show that the flame structure is correctly computed, images computed in the soot radiation band illustrate that the soot volume fraction is under predicted by the computations. The effect of the soot model and cause of under prediction is investigated further by correcting the soot volume fraction using an empirical state relationship. By comparing default simulations with computations using the state relation, it is shown that while the soot model under-estimates the soot concentration, it correctly computes the intermittency of soot in the flame. The study of sooting flames is extended further by performing a parametric analysis of physical and numerical parameters that affect soot formation and transport in two laboratory scale turbulent sooting flames, one fueled by natural gas and the other by ethylene. The study is focused on investigating the effect of molecular diffusion of species, dilution of fuel with hydrogen gas and the effect of chemical reaction mechanism on the soot concentration in the flame. The effect of species Lewis numbers on soot evolution and transport is investigated by carrying out simulations, first with the default equal diffusivity (ED) assumption and then by incorporating a differential diffusion (DD) model. Computations using the DD model over-estimate the concentration of the soot precursor and soot oxidizer species, leading to inconsistencies in the estimate of the soot concentration. The linear differential diffusion (LDD) model, reported previously to consistently model differential diffusion effects is implemented to correct the over prediction effect of the DD model. It is shown that the effect of species Lewis number on soot evolution is a secondary phenomenon and that soot is primarily transported by advection of the fluid in a turbulent flame. The effect of hydrogen dilution on the soot formation and transport process is also studied. It is noted that the decay of soot volume fraction and flame length with hydrogen addition follows trends observed in laminar sooting flame measurements. While hydrogen enhances mixing shown by the laminar flamelet solutions, the mixing effect does not significantly contribute to differential molecular diffusion effects in the soot nucleation regions downstream of the flame and has a negligible effect on soot transport. The sensitivity of computations of soot volume fraction towards the chemical reaction mechanism is shown. It is concluded that modeling reaction pathways of C3 and C4 species that lead up to Polycyclic Aromatic Hydrocarbon (PAH) molecule formation is paramount for accurate predictions of soot in the flame. (Abstract shortened by ProQuest.).

Controlling soot formation with filtered EGR for diesel and biodiesel fuelled engines.

PubMed

Gill, S S; Turner, D; Tsolakis, A; York, A P E

2012-04-03

Although exhaust gas recirculation (EGR) is an effective strategy for controlling the levels of nitrogen oxides (NO(X)) emitted from a diesel engine, the full potential of EGR in NO(X)/PM trade-off and engine performance (i.e., fuel economy) has not fully been exploited. Significant work into the cause and control of particulate matter (PM) has been made over the past decade with new cleaner fuels and after-treatment devices emerging to comply with the current and forthcoming emission regulations. In earlier work, we demonstrated that engine operation with oxygenated fuels (e.g., biodiesel) reduces the PM emissions and extends the engine tolerance to EGR before it reaches smoke-limited conditions. The same result has also been reported when high cetane number fuels such as gas-to-liquid (GTL) are used. To further our understanding of the relationship between EGR and PM formation, a diesel particulate filter (DPF) was integrated into the EGR loop to filter the recirculated soot particulates. The control of the soot recirculation penalty through filtered EGR (FEGR) resulted in a 50% engine-out soot reduction, thus showing the possibility of extending the maximum EGR limit or being able to run at the same level of EGR with an improved NO(X)/soot trade-off.

Fabrication of super-hydrophobic duo-structures

NASA Astrophysics Data System (ADS)

Zhang, X. Y.; Zhang, F.; Jiang, Y. J.; Wang, Y. Y.; Shi, Z. W.; Peng, C. S.

2015-04-01

Recently, super-hydrophobicity has attracted increasing attention due to its huge potential in the practical applications. In this paper, we have presented a duo-structure of the combination of micro-dot-matrix and nano-candle-soot. Polydimethylsiloxane (PDMS) was used as a combination layer between the dot-matrix and the soot particles. Firstly, a period of 9-μm dot-matrix was easily fabricated on the K9 glass using the most simple and mature photolithography process. Secondly, the dot-matrix surface was coated by a thin film of PDMS (elastomer: hardener=10:1) which was diluted by methylbenzene at the volume ratio of 1:8. Thirdly, we held the PDMS modified surface over a candle flame to deposit a soot layer and followed by a gentle water-risen to remove the non-adhered particles. At last, the samples were baked at 85°C for 2 hours and then the duo-structure surface with both micro-size dot-matrix and nano-size soot particles was obtained. The SEM indicated this novel surface morphology was quite like a lotus leaf of the well-know micro-nano-binary structures. As a result, the contact angle meter demonstrated such surface exhibited a perfect super-hydrophobicity with water contact angle of 153° and sliding angle of 3°. Besides, just listed as above, the fabrication process for our structure was quite more easy, smart and low-cost compared with the other production technique for super-hydrophobic surfaces such as the phase separation method, electrochemical deposition and chemical vapor deposition etc. Hence, this super-hydrophobic duo-structure reported in this letter was a great promising candidate for a wide and rapid commercialization in the future.

Experimental Investigation of Nascent Soot Physical Properties and The Influence on Particle Morphology and Growth

NASA Astrophysics Data System (ADS)

Lieb, Sydnie Marie

Soot released to the atmosphere is a dangerous pollutant for human health and the environment. Understanding the physical properties and surface properties of these particles is important to properly explaining the growth of soot particles in flames as well as their interactions with other particles and gases in the environment. Particles below 15 nm in diameter, nascent soot particles, dominate the early growth stages of soot formation; previously these particles were characterized as hard graphitic spheres. New evidence derived from the current dissertation work, to a large extent, challenges this prior characterization. This dissertation study begins by revisiting the use of atomic force microscope (AFM) as a tool to investigate the structural properties of nascent soot. The impact of tip artifacts, which are known to complicate measurements of features below 10 nm in diameter, are carefully considered so as to provide a concise interpretation of the morphology of nascent soot as seen by AFM. The results of the AFM morphology collaborate with earlier photo- and thermal-fragmentation particle mass spectrometry and Fourier transform infrared spectroscopy that nascent soot is not a graphitized carbon material and that they are not spherical. Furthermore, phase mode imaging is introduced as a method to investigate the physical properties of nascent soot particles in a greater detail and finer resolution. The helium ion microscope (HIM) has been identified as a useful technique for the imaging of nascent soot. Using this imaging method nascent soot particles were imaged with a high resolution that had not been obtained by prior techniques. The increased contrast provides a closer look at the nascent soot particles and further suggested that these particles are not as structurally homogeneous as previously thought. Geometric shape analysis was performed to characterize the particles in terms of sphericity, circularity, and fractal dimension. The geometric analysis showed that the particles deviate from spherical and that they are not characterized by a defined structure. This observation supports the theory that nascent soot is not homogenous in structure or composition, and challenges the classical assumption that spherical growth and aggregation are separate, size dependent processes. In light of the new evidence that suggests nascent soot particles are structurally inhomogenous, careful consideration must be given to mobility measurements of particle mass and size. The interpretation of particle volume of irregularly shaped nascent soot particles is considered in this dissertation work. Additionally, uncertainties in the mass density of nascent soot are reviewed and the error in mass calculation is quantified.

Sources and burial fluxes of soot black carbon in sediments on the Mackenzie, Chukchi, and Bering Shelves

NASA Astrophysics Data System (ADS)

Yang, Weifeng; Guo, Laodong

2018-03-01

Black carbon (BC) has been recognized as a climate forcing and a major component in the global carbon budget. However, studies on BC in the Arctic Ocean remain scarce. We report here variations in the abundance, sources and burial fluxes of sedimentary soot black carbon (soot-BC) in the western Arctic Ocean. The soot-BC contents averaged 1.6 ± 0.3, 0.46 ± 0.04 and 0.56 ± 0.10 mg-C g-1 on the Mackenzie, Chukchi and Bering Shelves, respectively, accounting for 16.6%, 10.2% and 10.4% of the total organic carbon in surface sediment. Temporally, contents of soot-BC remained fairly stable before 1910, but increased rapidly after the 1970s on the Mackenzie Shelf, indicating enhanced source input related to warming. Comparable δ13C signatures of soot-BC (- 24.95‰ to - 24.57‰) to C3 plants pointed to a major biomass source of soot-BC to the Beaufort Sea. Soot-BC showed similar temporal patterns with large fluctuations in the Chukchi/Bering shelf regions, implying the same source terms for soot-BC in these areas. Two events with elevated soot-BC corresponded to a simultaneous increase in biomass combustion and fossil fuel (coal and oil) consumption in Asia. The similar temporal variability in sedimentary soot-BC between the Arctic shelves and Asian lakes and the comparable δ13C values manifested that anthropogenic emission from East Asia was an important source of soot-BC in the western Arctic and subarctic regions. The burial fluxes of soot-BC, estimated from both 137Cs- and 210Pb-derived sedimentation rates, were 2.43 ± 0.42 g-C m-2 yr-1 on the Mackenzie Shelf, representing an efficient soot-BC sink. Soot-BC showed an increase in buried fluxes from 0.56 ± 0.02 g-C m-2 yr-1 during 1963-1986 to 0.88 ± 0.05 g-C m-2 yr-1 after 1986 on the Chukchi Shelf, and from 1.00 ± 0.18 g-C m-2 yr-1 to 2.58 ± 1.70 g-C m-2 yr-1 on the Bering Shelf, which were consistent with recent anthropogenically enhanced BC input observed especially in Asia. Overall, the three Arctic shelves could bury more than 3000 Gg soot-BC each year, attesting to an important role of the Arctic and subarctic shelves in global BC budget and carbon cycle.

Smoke Point in Co-flow Experiment

NASA Technical Reports Server (NTRS)

Urban, David L.; Sunderland, Peter B.; Yuan, Zeng-Guang

2009-01-01

The Smoke Point In Co-flow Experiment (SPICE) determines the point at which gas-jet flames (similar to a butane-lighter flame) begin to emit soot (dark carbonaceous particulate formed inside the flame) in microgravity. Studying a soot emitting flame is important in understanding the ability of fires to spread and in control of soot in practical combustion systems space. Previous experiments show that soot dominates the heat emitted from flames in normal gravity and microgravity fires. Control of this heat emission is critical for prevention of the spread of fires on Earth and in space for the design of efficient combustion systems (jet engines and power generation boilers). The onset of soot emission from small gas jet flames (similar to a butane-lighter flame) will be studied to provide a database that can be used to assess the interaction between fuel chemistry and flow conditions on soot formation. These results will be used to support combustion theories and to assess fire behavior in microgravity. The Smoke Point In Co-flow Experiment (SPICE) will lead to a o improved design of practical combustors through improved control of soot formation; o improved understanding of and ability to predict heat release, soot production and emission in microgravity fires; o improved flammability criteria for selection of materials for use in the next generation of spacecraft. The Smoke Point In Co-flow Experiment (SPICE) will continue the study of fundamental phenomena related to understanding the mechanisms controlling the stability and extinction of jet diffusion flames begun with the Laminar Soot Processes (LSP) on STS-94. SPICE will stabilize an enclosed laminar flame in a co-flowing oxidizer, measure the overall flame shape to validate the theoretical and numerical predictions, measure the flame stabilization heights, and measure the temperature field to verify flame structure predictions. SPICE will determine the laminar smoke point properties of non-buoyant jet diffusion flames (i.e., the properties of the largest laminar jet diffusion flames that do not emit soot) for several fuels under different nozzle diameter/co-flow velocity configurations. Luminous flame shape measurements would also be made to verify models of the flame shapes under co-flow conditions. The smoke point is a simple measurement that has been found useful to study the influence of flow and fuel properties on the sooting propensity of flames. This information would help support current understanding of soot processes in laminar flames and by analogy in turbulent flames of practical interest.

Neutron diffraction study of water freezing on aircraft engine combustor soot.

PubMed

Tishkova, V; Demirdjian, B; Ferry, D; Johnson, M

2011-12-14

The study of the formation of condensation trails and cirrus clouds on aircraft emitted soot particles is important because of its possible effects on climate. In the present work we studied the freezing of water on aircraft engine combustor (AEC) soot particles under conditions of pressure and temperature similar to the upper troposphere. The microstructure of the AEC soot was found to be heterogeneous containing both primary particles of soot and metallic impurities (Fe, Cu, and Al). We also observed various surface functional groups such as oxygen-containing groups, including sulfate ions, that can act as active sites for water adsorption. Here we studied the formation of ice on the AEC soot particles by using neutron diffraction. We found that for low amount of adsorbed water, cooling even up to 215 K did not lead to the formation of hexagonal ice. Whereas, larger amount of adsorbed water led to the coexistence of liquid water (or amorphous ice) and hexagonal ice (I(h)); 60% of the adsorbed water was in the form of ice I(h) at 255 K. Annealing of the system led to the improvement of the crystal quality of hexagonal ice crystals as demonstrated from neutron diffraction.

Black carbon radiative forcing at TOA decreased during aging.

PubMed

Wu, Yu; Cheng, Tianhai; Zheng, Lijuan; Chen, Hao

2016-12-05

During aging processing, black carbon (also called soot) particles may tend to be mixed with other aerosols, and highly influence their radiative forcing. In this study, freshly emitted soot particles were simulated as fractal aggregates composed of small spherical primary monomers. After aging in the atmosphere, soot monomers were coated by a thinly layer of sulfate as thinly coated soot particles. These soot particles were entirely embedded into large sulfate particle by further aging, and becoming heavily coated soot particles. In clear-sky conditions, black carbon radiative forcing with different aging states were investigated for the bottom and top of atmosphere (BOA and TOA). The simulations showed that black carbon radiative forcing increased at BOA and decreased at TOA after their aging processes. Thinly and heavily coated states increased up to ~12% and ~35% black carbon radiative forcing at BOA, and black carbon radiative forcing at TOA can reach to ~20% and ~100% smaller for thinly and heavily coated states than those of freshly emitted states, respectively. The effect of aging states of black carbon radiative forcing was varied with surface albedo, aerosol optical depth and solar zenith angles. These findings would be helpful for the assessments of climate change.

Effects of Chemical Aging on the Heterogeneous Freezing of Organic Aerosols

NASA Astrophysics Data System (ADS)

Collier, K.; Brooks, S. D.

2014-12-01

Organic aerosols are emitted into the atmosphere from a variety of sources and display a wide range of effectiveness in promoting the nucleation of ice in clouds. Soot and polycyclic aromatic hydrocarbons (PAHS) arise from incomplete combustion and other pollutant sources. Hydrocarbon compounds in diesel motor oil and other fuel blends include compounds such as octacosane (a straight saturated alkane), squalane (a branched saturated alkane) and squalene (an unsaturated branched alkene). At temperatures above -36°C, the formation of ice crystals in the atmosphere is facilitated by heterogeneous freezing processes in which atmospheric aerosols act as ice nuclei (IN). The variability in ability of organic particles to facilitate heterogeneous ice nucleation causes major uncertainties in predictions of aerosol effects on climate. Further, atmospheric aerosol composition and ice nucleation ability can be altered via chemical aging and reactions with atmospheric oxidants such as ozone. In this study, we take a closer look at the role of chemical oxidation on the efficiency of specific IN during contact freezing laboratory experiments. The freezing temperatures of droplets in contact with representative organic aerosols are determined through the use of an optical microscope apparatus equipped with a cooling stage and a digital camera. Chemical changes at the surface of aerosols due to ozone exposure are characterized using Raman Microspectroscopy and Fourier Transform Infrared Spectroscopy with Horizontal Attenuated Total Reflectance. Our results indicate that oxidation of certain atmospheric organics (soot and PAHS) enhances their ice nucleation ability. In this presentation, results of heterogeneous nucleation on various types of organic aerosols will be presented, and the role of structure in promoting freezing will be discussed.

Analysis for Mar Vel Black and acetylene soot low reflectivity surfaces for star tracker sunshade applications

NASA Technical Reports Server (NTRS)

Yung, E.

1974-01-01

Mar Vel Black is a revolutionary new extremely low reflectivity anodized coating developed by Martin Marietta of Denver. It is of great interest in optics in general, and in star trackers specifically because it can reduce extraneous light reflections. A sample of Mar Vel Black was evaluated. Mar Vel Black looks much like a super black surface with many small peaks and very steep sides so that any light incident upon the surface will tend to reflect many times before exiting that surface. Even a high reflectivity surface would thus appear to have a very low reflectivity under such conditions. Conversely, acetylene soot does not have the magnified surface appearance of a super black surface. Its performance is, however, predictable from the surface structure, considering the known configuration of virtually pure carbon.

Measurements and Modeling of Soot Formation and Radiation in Microgravity Jet Diffusion Flames. Volume 4

NASA Technical Reports Server (NTRS)

Ku, Jerry C.; Tong, Li; Greenberg, Paul S.

1996-01-01

This is a computational and experimental study for soot formation and radiative heat transfer in jet diffusion flames under normal gravity (1-g) and microgravity (0-g) conditions. Instantaneous soot volume fraction maps are measured using a full-field imaging absorption technique developed by the authors. A compact, self-contained drop rig is used for microgravity experiments in the 2.2-second drop tower facility at NASA Lewis Research Center. On modeling, we have coupled flame structure and soot formation models with detailed radiation transfer calculations. Favre-averaged boundary layer equations with a k-e-g turbulence model are used to predict the flow field, and a conserved scalar approach with an assumed Beta-pdf are used to predict gaseous species mole fraction. Scalar transport equations are used to describe soot volume fraction and number density distributions, with formation and oxidation terms modeled by one-step rate equations and thermophoretic effects included. An energy equation is included to couple flame structure and radiation analyses through iterations, neglecting turbulence-radiation interactions. The YIX solution for a finite cylindrical enclosure is used for radiative heat transfer calculations. The spectral absorption coefficient for soot aggregates is calculated from the Rayleigh solution using complex refractive index data from a Drude- Lorentz model. The exponential-wide-band model is used to calculate the spectral absorption coefficient for H20 and C02. It is shown that when compared to results from true spectral integration, the Rosseland mean absorption coefficient can provide reasonably accurate predictions for the type of flames studied. The soot formation model proposed by Moss, Syed, and Stewart seems to produce better fits to experimental data and more physically sound than the simpler model by Khan et al. Predicted soot volume fraction and temperature results agree well with published data for a normal gravity co-flow laminar flames and turbulent jet flames. Predicted soot volume fraction results also agree with our data for 1-g and 0-g laminar jet names as well as 1-g turbulent jet flames.

Quantitative analysis of in situ optical diagnostics for inferring particle/aggregate parameters in flames: Implications for soot surface growth and total emissivity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koeylue, U.O.

1997-05-01

An in situ particulate diagnostic/analysis technique is outlined based on the Rayleigh-Debye-Gans polydisperse fractal aggregate (RDG/PFA) scattering interpretation of absolute angular light scattering and extinction measurements. Using proper particle refractive index, the proposed data analysis method can quantitatively yield all aggregate parameters (particle volume fraction, f{sub v}, fractal dimension, D{sub f}, primary particle diameter, d{sub p}, particle number density, n{sub p}, and aggregate size distribution, pdf(N)) without any prior knowledge about the particle-laden environment. The present optical diagnostic/interpretation technique was applied to two different soot-containing laminar and turbulent ethylene/air nonpremixed flames in order to assess its reliability. The aggregate interpretationmore » of optical measurements yielded D{sub f}, d{sub p}, and pdf(N) that are in excellent agreement with ex situ thermophoretic sampling/transmission electron microscope (TS/TEM) observations within experimental uncertainties. However, volume-equivalent single particle models (Rayleigh/Mie) overestimated d{sub p} by about a factor of 3, causing an order of magnitude underestimation in n{sub p}. Consequently, soot surface areas and growth rates were in error by a factor of 3, emphasizing that aggregation effects need to be taken into account when using optical diagnostics for a reliable understanding of soot formation/evolution mechanism in flames. The results also indicated that total soot emissivities were generally underestimated using Rayleigh analysis (up to 50%), mainly due to the uncertainties in soot refractive indices at infrared wavelengths. This suggests that aggregate considerations may not be essential for reasonable radiation heat transfer predictions from luminous flames because of fortuitous error cancellation, resulting in typically a 10 to 30% net effect.« less

Killer smog of London, 50 years on: particle properties and oxidative capacity.

PubMed

Whittaker, Andy; BéruBé, Kelly; Jones, Tim; Maynard, Robert; Richards, Roy

2004-12-01

Total suspended particulate (TSP) samples collected on glass fibre filters in London before (1955) and after (1958-1974) the Clean Air Act was examined for physicochemical characteristics and oxidative capacity. High-resolution microscopy identified most of the material as soot with smelter spheres, fly ash (FA), sodium chloride and calcium sulphate particles. Image analysis (IA) was used to show that most of the soot aggregates were less than 1 microm in size and contained chains of individual particles of 10-50 nm. Speed mapping of large agglomerates of the historic particles confirmed that the samples were enriched with soot probably derived from a sulphur-rich coal called nutty slack which was used extensively at this time. Inductively coupled plasma-mass spectrometry (ICP-MS) was used to examine elemental composition. Meaningful quantitation of certain elements (Mg, Al and Zn) proved impossible because they were in high quantities in the glass fibre filters. However, high quantities of Fe>Pb>Cu>Mn>V>As were detected which may explain in part the bioreactivity of the samples. Using a simple in vitro test of oxidative capacity (plasmid assay), one historic particulate sample (1958) showed three times the activity of a modern-day diesel exhaust particle (DEP) sample but ten times less activity than a modern-day urban ambient particle collection. Such studies are continuing to link particle physicochemical properties and bioreactivity with a wider range of the samples collected between 1955 and 74 and how such historic samples compare with present-day London ambient particles.

Investigating isotopic signatures of atmospheric nitrous acid (HONO)

NASA Astrophysics Data System (ADS)

Chai, J.; Miller, D. J.; Hastings, M. G.

2016-12-01

Nitrous acid (HONO) is an important reactive nitrogen species that can be easily photolyzed to nitrogen oxide and hydroxyl radical in the troposphere. HONO greatly influences atmospheric oxidation capacity, affecting the formation of tropospheric ozone (O3) and secondary aerosol. Recent studies have indicated that in addition to heterogeneous NOx reactions, biomass burning, soil emission and photolysis of nitric acid (HNO3) on surfaces (e.g. aerosol particles and soot) are also important sources of HONO. However, these sources have not yet been well constrained. The stable isotope ratios in nitrate have been successfully used to trace NOx sources and oxidation chemistry in the atmosphere. Can the isotopic signatures of HONO be used to trace NOx oxidation and renoxification pathways? For this purpose, we have built an annular denuder HONO collection system for the stable isotope study of HONO. Preliminary tests show successful collection and recovery of HONO synthesized in our lab. Nitrogen and oxygen isotopic analysis of the recovered HONO also shows consistent isotopic signatures. Results from field applications of this method in near road and on road environments, agricultural settings, and laboratory based biomass burns will be presented.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew T.

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfatemore » mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveT gand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibitmore » a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.« less

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation

DOE PAGES

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew; ...

2017-01-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibitmore » a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.« less

Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation

DOE PAGES

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew T.; ...

2017-01-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfatemore » mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveT gand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.« less

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation.

PubMed

Charnawskas, Joseph C; Alpert, Peter A; Lambe, Andrew T; Berkemeier, Thomas; O'Brien, Rachel E; Massoli, Paola; Onasch, Timothy B; Shiraiwa, Manabu; Moffet, Ryan C; Gilles, Mary K; Davidovits, Paul; Worsnop, Douglas R; Knopf, Daniel A

2017-08-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles' organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g ) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.

Interaction of SO{sub x} and NO{sub x} with soot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chughtai, A.R.; Atteya, M.M.O.; Konowalchuk, B.K.

1996-12-31

As part of a continuing study of the heterogeneous reactions of black carbon with gas phase oxidant species, the adsorption of low concentrations (30 - 2000 ppm) of so, and NO{sub 2} individually, together, and in the presence of other adsorbates have been studied by spectroscopic and microgravimetric techniques. Previous work in this study has revealed a dual path mechanism for the reaction of NO{sub 2}/N{sub 2}O{sub 4} with n-hexane soot over concentration range 9 ppm - 200 torr. (This soot has been used throughout these investigations as a model for fossil fuel-produced black carbon). Interaction of SO{sub 2} andmore » carbon represent the most intensively studied of the heterogeneous systems containing carbon. An attempt to understand the molecular dynamics involved in the reactions of carbon in the presence of multiple reactants, such as SO{sub 2} and NO{sub 2}, underlies the present work.« less

Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles.

PubMed

China, Swarup; Mazzoleni, Claudio; Gorkowski, Kyle; Aiken, Allison C; Dubey, Manvendra K

2013-01-01

Biomass burning is one of the largest sources of carbonaceous aerosols in the atmosphere, significantly affecting earth's radiation budget and climate. Tar balls, abundant in biomass burning smoke, absorb sunlight and have highly variable optical properties, typically not accounted for in climate models. Here we analyse single biomass burning particles from the Las Conchas fire (New Mexico, 2011) using electron microscopy. We show that the relative abundance of tar balls (80%) is 10 times greater than soot particles (8%). We also report two distinct types of tar balls; one less oxidized than the other. Furthermore, the mixing of soot particles with other material affects their optical, chemical and physical properties. We quantify the morphology of soot particles and classify them into four categories: ~50% are embedded (heavily coated), ~34% are partly coated, ~12% have inclusions and~4% are bare. Inclusion of these observations should improve climate model performances.

Investigation of Sooting in Microgravity Droplet Combustion: Fuel-Dependent Effects

NASA Technical Reports Server (NTRS)

Manzello, Samuel L.; Hua, Ming; Choi, Mun Young

1999-01-01

Kumagai and coworkers first performed microgravity droplet combustion experiments [Kumagai, 1957]. The primary goal of these early experiments were to validate simple 'd(sup 2)-law models [Spalding, 1954, Godsave, 1954] Inherent in the 'd(sup 2) -law' formulation and in the scope of the experimental observation is the neglect of sooting behavior. In fact, the influence of sooting has not received much attention until more recent works [Choi et al., 1990; Jackson et al., 1991; Jackson and Avedisian, 1994; Choi and Lee, 1996; Jackson and Avedisian, 1996; Lee et al., 1998]:. Choi and Lee measured soot volume fraction for microgravity droplet flames using full-field light extinction and subsequent tomographic inversion [Choi and Lee, 1996]. In this investigation, soot concentrations were measured for heptane droplets and it was reported that soot concentrations were considerably higher in microgravity compared to the normal gravity flame. It was reasoned that the absence of buoyancy and the effects of thermophoresis resulted in the higher soot concentrations. Lee et al. [1998] performed soot measurement experiments by varying the initial droplet diameter and found marked influence of sooting on the droplet burning behavior. There is growing sentiment that sooting in droplet combustion must no longer be neglected and that "perhaps one of the most important outstanding contributions of (micro)g droplet combustion is the observation that in the absence of asymmetrical forced and natural convection, a soot shell is formed between the droplet surface and the flame, exerting an influence on the droplet combustion response far greater than previously recognized." [Law and Faeth, 1994]. One of the methods that we are exploring to control the degree of sooting in microgravity is to use different fuels. The effect of fuel structure on sooting propensity has been investigated for over-ventilated concentric coflowing buoyant diffusion flames. (Glassman, 1996]. In these investigations, the fuel flowrate was increased until smoke was observed to escape from the "luminous visible flame" [Glassman, 1996]. A total of 29 fuels were used in order to characterize relative sooting propensity. The sooting propensity of a particular fuel was assessed by comparing the flowrates for soot emission from the tip of the flame. It was reported that the sooting tendency for diffusion flames increased for fuels with higher rates of pyrolysis. Randolph and Law [1986 and not 1994] also examined the effect of fuel structure on droplet sooting behavior. In their experiments the droplets were separated from the bulk gas stream and quenched with nitrogen prior to gravimetric measurements. A variety of fuels were studied, namely aromatics, phenyl-alkanes and alkanes. The results were in qualitative agreement with the work of Glassman [1986]. Vander Wal et al. [1994] performed relative soot concentration measurements using laser-induced incandescence for heptane and decane fuel droplets burning under normal-gravity conditions. It was found that soot volume fractions for decane was more than a factor of two larger than that for heptane. Although the normal-gravity investigations have provided some important insights regarding the influence of fuel structure on the sooting behavior of droplet flames, results cannot be easily extrapolated for microgravity studies since increased residence times and thermophoretic effects must be considered in greater detail. Several studies have compared sooting behavior of different fuel droplets burning under microgravity conditions [Card and Choi, 1990; Jackson et al., 1991; Jackson and Avedisian, 1994], however, detailed quantitative results were not provided. In all of these previous studies, the degree of sooting was only visually assessed from an incandescent backlighted image of the soot containing region. Such techniques can provide misleading results regarding sooting behavior [Choi, 1996].

Soot climate forcing via snow and ice albedos.

PubMed

Hansen, James; Nazarenko, Larissa

2004-01-13

Plausible estimates for the effect of soot on snow and ice albedos (1.5% in the Arctic and 3% in Northern Hemisphere land areas) yield a climate forcing of +0.3 W/m(2) in the Northern Hemisphere. The "efficacy" of this forcing is approximately 2, i.e., for a given forcing it is twice as effective as CO(2) in altering global surface air temperature. This indirect soot forcing may have contributed to global warming of the past century, including the trend toward early springs in the Northern Hemisphere, thinning Arctic sea ice, and melting land ice and permafrost. If, as we suggest, melting ice and sea level rise define the level of dangerous anthropogenic interference with the climate system, then reducing soot emissions, thus restoring snow albedos to pristine high values, would have the double benefit of reducing global warming and raising the global temperature level at which dangerous anthropogenic interference occurs. However, soot contributions to climate change do not alter the conclusion that anthropogenic greenhouse gases have been the main cause of recent global warming and will be the predominant climate forcing in the future.

Significant Climate Changes Caused by Soot Emitted From Rockets in the Stratosphere

NASA Astrophysics Data System (ADS)

Mills, M. J.; Ross, M.; Toohey, D. W.

2010-12-01

A new type of hydrocarbon rocket engine with a larger soot emission index than current kerosene rockets is expected to power a fleet of suborbital rockets for commercial and scientific purposes in coming decades. At projected launch rates, emissions from these rockets will create a persistent soot layer in the northern middle stratosphere that would disproportionally affect the Earth’s atmosphere and cryosphere. A global climate model predicts that thermal forcing in the rocket soot layer will cause significant changes in the global atmospheric circulation and distributions of ozone and temperature. Tropical ozone columns decline as much as 1%, while polar ozone columns increase by up to 6%. Polar surface temperatures rise one Kelvin regionally and polar summer sea ice fractions shrink between 5 - 15%. After 20 years of suborbital rocket fleet operation, globally averaged radiative forcing (RF) from rocket soot exceeds the RF from rocket CO_{2} by six orders of magnitude, but remains small, comparable to the global RF from aviation. The response of the climate system is surprising given the small forcing, and should be investigated further with different climate models.

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

NASA Astrophysics Data System (ADS)

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 the volume equivalent diameter of soot agglomerate containing internal voids and calculated in-situ dynamic shape factor. Our study is the first study that tracks in situ microphysical changes in soot morphology quantitatively, providing the detailed status of both fresh and coated soot particles.

Physico-Chemical Characterization of Fine and Ultrafine Particles Emitted during Diesel Particulate Filter Active Regeneration of Euro5 Diesel Vehicles.

PubMed

R'Mili, Badr; Boréave, Antoinette; Meme, Aurelie; Vernoux, Philippe; Leblanc, Mickael; Noël, Ludovic; Raux, Stephane; D'Anna, Barbara

2018-03-06

Diesel particulate filters (DPFs) are commonly employed in modern passenger cars to comply with current particulate matter (PM) emission standards. DPFs requires periodic regeneration to remove the accumulated matter. During the process, high-concentration particles, in both nucleation and accumulation modes, are emitted. Here, we report new information on particle morphology and chemical composition of fine (FPs) and ultrafine particles (UFPs) measured downstream of the DPF during active regeneration of two Euro 5 passenger cars. The first vehicle was equipped with a close-coupled diesel oxidation catalyst (DOC) and noncatalyzed DPF combined with fuel borne catalyst and the second one with DOC and a catalyzed-diesel particle filter (CDPF). Differences in PM emission profiles of the two vehicles were related to different after treatment design, regeneration strategies, and vehicle characteristics and mileage. Particles in the nucleation mode consisted of ammonium bisulfate, sulfate and sulfuric acid, suggesting that the catalyst desulfation is the key process in the formation of UFPs. Larger particles and agglomerates, ranging from 90 to 600 nm, consisted of carbonaceous material (soot and soot aggregates) coated by condensable material including organics, ammonium bisulfate and sulfuric acid. Particle emission in the accumulation mode was due to the reduced filtration efficiency (soot cake oxidation) throughout the regeneration process.

Laboratory Studies of Heterogeneous Chemical Processes of Atmospheric Importance

NASA Technical Reports Server (NTRS)

Molina, Mario J.

2003-01-01

The objective of this study is to conduct measurements of chemical kinetics parameters for heterogeneous reactions of importance in the stratosphere and the troposphere. It involves the elucidation of the mechanism of the interaction of HC1 vapor with ice surfaces, which is the first step in the heterogeneous chlorine activation processes, as well as the investigation of the atmospheric oxidation mechanism of soot particles emitted by biomass and fossil fuels. The techniques being employed include turbulent flow- chemical ionization mass spectrometry and optical ellipsometry, among others. The next section summarizes our research activities during the first year of the project, and the section that follows consists of the statement of work for the second year.

COSMIC: Carbon Monoxide and Soot in Microgravity Inverse Combustion

NASA Technical Reports Server (NTRS)

Blevins, L. G.; Fernandez, M. G.; Mulholland, G. W.; Davis, R. W.; Moore, E. F.; Steel, E. B.; Scott, J. H. J.

2001-01-01

Almost seventy percent of deaths in accidental fires are caused by inhalation of toxins such as carbon monoxide (CO) and smoke (soot) that form during underventilated burning. The COSMIC project examines the formation mechanisms of CO and soot during underventilated combustion, achieved presently using laminar, inverse diffusion flames (IDFs) formed between an air jet and surrounding fuel. A major hypothesis of the project is that the IDF mimics underventilated combustion because carbon-containing species that form on the fuel side of the flame (such as CO and soot) can escape without passing through an oxidizing flame tip. An IDF literature review was presented at the last microgravity workshop, and a few additional IDF papers have appeared since that meeting. The COSMIC project is entering the third year of its four-year funding cycle. The first two years have been devoted to designing and constructing a rig for use in the NASA 2.2-second drop tower. A few computations and laboratory experiments have been performed. The goals of this paper are to discuss the use of numerical simulation during burner design, to present computational and experimental results that support the hypothesis that IDFs are similar to underventilated flames, and to delineate future plans.

Light absorbing material (soot) in rainwater and in aerosol particles in the Maldives

NASA Astrophysics Data System (ADS)

Granat, L.; EngströM, J. E.; Praveen, S.; Rodhe, H.

2010-08-01

Simultaneous measurements of soot (absorbing material at 528 nm) and inorganic ions in aerosol and precipitation at the Maldives Climate Observatory Hanimaadhoo during the period May 2005 to February 2007 have made it possible to calculate the washout ratio (WR) of these components as a measure of how efficiently they are scavenged by precipitation. On the basis of air trajectories the data have been separated into days with polluted air arriving from the Indian subcontinent in a northeasterly sector during winter and clean monsoon days with southerly flow from the Indian Ocean. The average soot concentration was a factor of 10 higher in the former situations. Despite considerable scatter for individual days, a systematic pattern emerged when the WR for the different components were compared with each other. During the monsoon season the WR for soot was similar to that of sulfate and other fine mode aerosol components, indicating that soot containing particles in these situations were efficient as cloud condensation nuclei. The origin of the light absorbing material during the monsoon season is unclear. During the polluted winter days, on the other hand, the WR for soot was three times smaller than that of sulfate. This indicates that, even after a travel time of several days, the soot containing particles from India have retained much of their hydrophobic property. The low WR and the infrequent rain during this season probably contribute to extending the atmospheric lifetime of soot well beyond several days. Surprisingly high concentrations of non-sea-salt calcium were measured during the monsoon season, substantially higher than during the winter season. The origin of these high values could be long-range transport from the Australian or African continents. Another possibility might be exopolymer gels derived from the ocean surface microlayer.

Spectral Signature of Radiative Forcing by East Asian Dust-Soot Mixture

NASA Astrophysics Data System (ADS)

Zhu, A.; Ramanathan, V.

2007-12-01

The Pacific Dust Experiment (PACDEX) provides the first detailed sampling of dust-soot mixtures from the western Pacific to the eastern Pacific Ocean. The data includes down and up spectral irradiance, mixing state of dust and soot, and other aerosol properties. This study attempts to simulate the radiative forcing by dust-soot mixtures during the experimental period. The MODTRAN band model was employed to investigate the spectral signatures of solar irradiance change induced by aerosols at moderate spectral resolutions. For the short wave band (300-1100nm) used in this study, the reduction of downward irradiance at surface by aerosols greatly enhances with increasing wavelength in the UV band (300-400nm), reaches a maximum in the blue band, then gradually decreases toward the red band. In the near-IR band (700-1100nm), irradiance reduction by aerosols shows great fluctuations in the band with center wavelength at around 940nm, 820nm, 720nm, 760nm, 690nm, where the aerosol effect is overwhelmed by the water vapor and O2 absorptions. The spectral pattern of irradiance reduction varies for different aerosol species. The maximum reduction lies at around 450nm for soot, and shifting to about 490nm for East Asian mineral dust. It's worth noting that although soot aerosols reduce more irradiance than East Asian dust in the UV and blue band, the impact of dust to the irradiance exceeds that by soot at the longer wavelength band (i.e. around 550nm). The reduction of irradiance by East Asian dust (soot) in the UV band, visible band, and near-IR accounts for about 6% (10%), 56% (64%), and 38% (26%) of total irradiance reduction. As large amount of soot aerosols are involved during the long range transport of East Asian dust, the optical properties of dust aerosols are modified with different mixing state with soot, the spectral pattern of the irradiance reduction will be changed. The study of aerosol forcing at moderate spectral resolutions has the potential application for research on aerosol mixing state and its climate impacts.

Development and applications of laser-induced incandescence

NASA Technical Reports Server (NTRS)

Vanderwal, Randy L.; Dietrich, Daniel L.; Zhou, Zhiquang; Choi, Mun Y.

1995-01-01

Several NASA-funded investigations focus on soot processes and radiative influences of soot in diffusion flames given their simplicity, practical significance, and potential for theoretical modeling. Among the physical parameters characterizing soot, soot volume fraction, f(sub v), a function of particle size and number density, is often of chief practical interest in these investigations, as this is the geometrical property that directly impacts radiative characteristics and the temperature field of the flame and is basic to understanding soot growth and oxidation processes. Diffusion flames, however, present a number of challenges to the determination of f(sub v) via traditional extinction measurements. Laser-induced incandescence (LII) possesses several advantages compared to line-of-sight extinction techniques for determination of f(sub v). Since LII is not a line-of-sight technique, similar to fluorescence, it possesses geometric versatility allowing spatially resolved measurements of f(sub v) in real time in nonaxisymmetric systems without using deconvolution techniques. The spatial resolution of LII is determined by the detector and imaging magnification used. Neither absorption by polycyclic aromatic hydrocarbons (PAH's) nor scattering contributes to the signal. Temporal capabilities are limited only by the laser pulse and camera gate duration, with measurements having been demonstrated with 10 ns resolution. Because of these advantages, LII should be applicable to a variety of combustion processes involving both homogeneous and heterogeneous phases. Our work has focussed on characterization of the technique as well as exploration of its capabilities and is briefly described.

Experimental investigation of submicron and ultrafine soot particle removal by tree leaves

NASA Astrophysics Data System (ADS)

Hwang, Hee-Jae; Yook, Se-Jin; Ahn, Kang-Ho

2011-12-01

Soot particles emitted from vehicles are one of the major sources of air pollution in urban areas. In this study, five kinds of trees were selected as Pinus densiflora, Taxus cuspidata, Platanus occidentalis, Zelkova serrata, and Ginkgo biloba, and the removal of submicron (<1 μm) and ultrafine (<0.1 μm) soot particles by tree leaves was quantitatively compared in terms of deposition velocity. Soot particles were produced by a diffusion flame burner using acetylene as the fuel. The sizes of monodisperse soot particles classified with the Differential Mobility Analyzers (DMA) were 30, 55, 90, 150, 250, 400, and 600 nm. A deposition chamber was designed to simulate the omni-directional flow condition around the tree leaves. Deposition velocities onto the needle-leaf trees were higher than those onto the broadleaf trees. P. densiflora showed the greatest deposition velocity, followed by T. cuspidata, Platanus occidentalis, Zelkova serrata, and Ginkgo biloba. In addition, from the comparison of deposition velocity between two groups of Platanus occidentalis leaves, i.e. one group of leaves with front sides only and the other with back sides only, it was supposed in case of the broadleaf trees that the removal of airborne soot particles of submicron and ultrafine sizes could be affected by the surface roughness of tree leaves, i.e. the veins and other structures on the leaves.

In-situ neutron imaging of hydrogenous fuels in combustion generated porous carbons under dynamic and steady state pressure conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ossler, Frederik; Santodonato, Louis J.; Bilheux, Hassina Z.

Here, we report results from experiments where we characterize the surface properties of soot particles interacting with high-pressure methane. We also found considerable differences in behavior of the soot material between static and dynamic pressure conditions that can be explained by multiscale correlations in the dynamics, from the micro to macro of the porous fractal-like carbon matrix. The measurements were possible utilizing cold neutron imaging of methane mixed with combustion generated carbon (soot) inside steel cells. The studies were performed under static and dynamic pressure conditions in the range 10-90 bar, and are of interest for applications of energy storagemore » of hydrogenous fuels. The very high cross sections for neutrons compared to hard X-ray photons, enabled us to find considerable amounts of native hydrogen in the soot and to see and quantify the presence of hydrogen atoms in the carbon soot matrix under different pressure conditions. Our work lays the base for more detailed in-situ investigations on the interaction of porous carbon materials with hydrogen in practical environments for hydrogen and methane storage.« less

In-situ neutron imaging of hydrogenous fuels in combustion generated porous carbons under dynamic and steady state pressure conditions

DOE PAGES

Ossler, Frederik; Santodonato, Louis J.; Bilheux, Hassina Z.

2017-02-12

Here, we report results from experiments where we characterize the surface properties of soot particles interacting with high-pressure methane. We also found considerable differences in behavior of the soot material between static and dynamic pressure conditions that can be explained by multiscale correlations in the dynamics, from the micro to macro of the porous fractal-like carbon matrix. The measurements were possible utilizing cold neutron imaging of methane mixed with combustion generated carbon (soot) inside steel cells. The studies were performed under static and dynamic pressure conditions in the range 10-90 bar, and are of interest for applications of energy storagemore » of hydrogenous fuels. The very high cross sections for neutrons compared to hard X-ray photons, enabled us to find considerable amounts of native hydrogen in the soot and to see and quantify the presence of hydrogen atoms in the carbon soot matrix under different pressure conditions. Our work lays the base for more detailed in-situ investigations on the interaction of porous carbon materials with hydrogen in practical environments for hydrogen and methane storage.« less

Efficient low-temperature soot combustion by bimetallic Ag-Cu/SBA-15 catalysts.

PubMed

Wen, Zhaojun; Duan, Xinping; Hu, Menglin; Cao, Yanning; Ye, Linmin; Jiang, Lilong; Yuan, Youzhu

2018-02-01

In this study, the effects of copper (Cu) additive on the catalytic performance of Ag/SBA-15 in complete soot combustion were investigated. The soot combustion performance of bimetallic Ag-Cu/SBA-15 catalysts was higher than that of monometallic Ag and Cu catalysts. The optimum catalytic performance was acquired with the 5Ag 1 -Cu 0.1 /SBA-15 catalyst, on which the soot combustion starts at T ig =225°C with a T 50 =285°C. The temperature for 50% of soot combustion was lower than that of conventional Ag-based catalysts to more than 50°C (Aneggi et al., 2009). Physicochemical characterizations of the catalysts indicated that addition of Cu into Ag could form smaller bimetallic Ag-Cu nanolloy particles, downsizing the mean particle size from 3.7nm in monometallic catalyst to 2.6nm in bimetallic Ag-Cu catalyst. Further experiments revealed that Ag and Cu species elicited synergistic effects, subsequently increasing the content of surface active oxygen species. As a result, the structure modifications of Ag by the addition of Cu strongly intensified the catalytic performance. Copyright © 2017. Published by Elsevier B.V.

Phototransformation Rate Constants of PAHs Associated with Soot Particles

PubMed Central

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 (k0p), the effective diffusion coefficients (Deff), and the light penetration depths (z0.5) 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 z0.5 is more sensitive to the soot layer thickness than the k0p value. As the thickness of the soot layer increases, the z0.5 values increase, but the k0p 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 k0p and z0.5 in thinner layers, Deff 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. PMID:23247292

Direct numerical simulations of temporally developing hydrocarbon shear flames at elevated pressure: effects of the equation of state and the unity Lewis number assumption

NASA Astrophysics Data System (ADS)

Korucu, Ayse; Miller, Richard

2016-11-01

Direct numerical simulations (DNS) of temporally developing shear flames are used to investigate both equation of state (EOS) and unity-Lewis (Le) number assumption effects in hydrocarbon flames at elevated pressure. A reduced Kerosene / Air mechanism including a semi-global soot formation/oxidation model is used to study soot formation/oxidation processes in a temporarlly developing hydrocarbon shear flame operating at both atmospheric and elevated pressures for the cubic Peng-Robinson real fluid EOS. Results are compared to simulations using the ideal gas law (IGL). The results show that while the unity-Le number assumption with the IGL EOS under-predicts the flame temperature for all pressures, with the real fluid EOS it under-predicts the flame temperature for 1 and 35 atm and over-predicts the rest. The soot mass fraction, Ys, is only under-predicted for the 1 atm flame for both IGL and real gas fluid EOS models. While Ys is over-predicted for elevated pressures with IGL EOS, for the real gas EOS Ys's predictions are similar to results using a non-unity Le model derived from non-equilibrium thermodynamics and real diffusivities. Adopting the unity Le assumption is shown to cause misprediction of Ys, the flame temperature, and the mass fractions of CO, H and OH.

Preliminary Assessment Of The Burning Dynamics Of Jp8 Droplets In Microgravity

NASA Technical Reports Server (NTRS)

Bae, J. H.; Avedisian, C. T.

2003-01-01

In this report we present new data for fuel droplet combustion in microgravity to examine the influence of ambient gas and fuel composition on flame structure and sooting dynamics for droplets with initial diameters in the range of 0.4mm to 0.5mm. The fuels are JP8 (a kerosene derivative) and nonane. The ambient gas is air and a mixture of 30% oxygen and 70% helium, the latter having been examined for burning under conditions where soot formation is minimal. Some data at elevated pressures are also reported. The burning process shows a nonlinear D2 progression which is independent of soot formation as burning in a helium inert showed the same nonlinear trend. Flames were proportionally farther from the droplet surface in helium than they were in air. A nondimensional parameter is presented that consolidates the three standoff distances for the droplet, flame and soot shell diameters within the initial diameter ranges examined.

Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol

DOE PAGES

Shrivastava, Manish; Lou, Silja; Zelenyuk, Alla; ...

2017-01-23

Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on ecosystems and human health. Laboratory measurements show that one of the most carcinogenic PAHs, benzo(a)pyrene, which is adsorbed on surfaces of soot particles, reacts very quickly with atmospheric oxidants like ozone within ~2 hours. Yet, field observations indicate that it actually persists for much longer periods in the atmosphere, and this large discrepancy is not well understood. Driven by novel experimental understanding, we develop a new modelling approach, whereby particle-bound BaP is shielded from oxidation by a coating of viscous organic aerosol (OA). We show that application of this new approach inmore » a global climate model leads to higher atmospheric BaP concentrations that agree much better with measurements, compared to the default model, as well as stronger long-range transport and greater deposition fluxes. Here, this new approach also predicts elevated lung-cancer risk from PAHs. Predicted oxidation of BaP is highest over a tropical belt where OA is liquid-like.« less

Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shrivastava, Manish; Lou, Silja; Zelenyuk, Alla

2017-01-23

Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on ecosystems and human health. Laboratory measurements show that one of the most carcinogenic PAHs, benzo(a)pyrene, which is adsorbed on surfaces of soot particles, reacts very quickly with atmospheric oxidants like ozone within ~2 hours. Yet, field observations indicate that it actually persists for much longer periods in the atmosphere, and this large discrepancy is not well understood. Driven by novel experimental understanding, we develop a new modelling approach, whereby particle-bound BaP is shielded from oxidation by a coating of viscous organic aerosol (OA). We show that application of this new approach inmore » a global climate model leads to higher atmospheric BaP concentrations that agree much better with measurements, compared to the default model, as well as stronger long-range transport and greater deposition fluxes. This new approach also predicts elevated lung-cancer risk from PAHs. Predicted oxidation of BaP is highest over a tropical belt where OA is liquid-like.« less

Kinetics and Structure of Superagglomerates Produced by Silane and Acetylene

NASA Technical Reports Server (NTRS)

Mulholland, G. W.; Hamins, A.; Sivathanu, Y.

1999-01-01

The evolution of smoke in a laminar diffusion flame involves several steps. The first step is particle inception/nucleation in the high-temperature fuel-rich region of the flame followed by surface growth and coagulation/coalescence of the small particles. As the primary spheres grow in size and lose hydrogen, the colliding particles no longer coalesce but retain their identity as a cluster of primary spheres, termed an agglomerate. Finally, in the upper portion of the flame, the particles enter an oxidizing environment which may lead to partial or complete burnout of the agglomerates. Currently there is no quantitative model for describing the growth of smoke agglomerates up to superagglomerates with an overall dimension of 10 microns and greater. Such particles are produced during the burning of acetylene and fuels containing benzene rings such as toluene and polystyrene. In the case of polystyrene, smoke agglomerates in excess of 1 mm have been observed "raining" out from large fires. Evidence of the formation of superagglomerates in a laminar acetylene/air diffusion flame has been recently reported. Acetylene was chosen as the fuel since the particulate loading in acetylene/air diffusion flames is very high. Photographs were obtained by Sorensen using a microsecond xenon lamp of the "stream" of soot just above the flame. For low flow rates of acetylene, only submicrometer soot clusters are produced and they give rise to the homogeneous appearance of the soot stream. When the flow rate is increased to 1.7 cu cm/s, soot clusters up to 10 microns are formed and they are responsible for the graininess and at a flow rate of 3.4 cu cm/s, a web of interconnected clusters as large as the width of the flame is seen. This interconnecting web of superagglomerates is described as a gel state by Sorensen et al (1998). This is the first observation of a gel for a gas phase system. It was observed that this gel state immediately breaks up into agglomerates due to buoyancy induced turbulence and gravitational sedimentation.

Distribution, Transport, and Accumulation of Pyrogenic Black Carbon in Post-Wildfire Watersheds

NASA Astrophysics Data System (ADS)

Galanter, A.; Cadol, D. D.; Frey, B.; Lohse, K. A.

2014-12-01

Large, high severity wildfires greatly alter forest structure, water quality, and soil development/erosion. With increased frequency of such wildfires also follows heavy post-wildfire debris flows and flooding which deliver high loads of sediment and pyrogenic black carbon (PyC) to downstream waterways. The accumulation of PyC is a multi-faceted and dynamic issue in the critical zone. Generated by incomplete combustion of organic matter, PyC (in the form of soot and char) impacts turbidity, biological and chemical oxygen demand, and pH. In addition, PyC has the potential to sequester contaminants and can store carbon over short and long timescales. The impacts of two recent wildfires in Northern New Mexico are studied with the goal of understanding the fluxes and residence times of PyC in post-wildfire, mountainous watersheds. Employing burn severity maps and geospatial data, we selected three sites to collect soil and water samples to characterize PyC: a control, an area impacted by a large, severe burn (2011), and an area impacted by a smaller, less severe burn (2013). By collaborating with researchers at the Jemez Critical Zone Observatory, soil samples are being analyzed and will provide pre-wildfire PyC concentrations for the 2013 burn area. In this study, PyC is treated as both a particulate and a solute that is transported throughout the watershed as well as degraded in soils, surface water and groundwater. We used two black carbon quantification methods: the chemo-thermal oxidation (CTO-375) method to distinguish between soil soot and char, and the benzene polycarboxylic acids (BPCA) method to quantify the total concentrations of PyC in soil and water samples. Preliminary soil data from the CTO-375 method show comparable soot concentrations in the control, 2011, and 2013 burn indicating that the soot is more recalcitrant than char and remains in the watershed long after a wildfire. This data also suggests that the fluxes of black carbon over short time scales are composed mainly of char.

An experimental and theoretical study of radiative extinction of diffusion flames

NASA Technical Reports Server (NTRS)

Wichman, Indrek S.; Atreya, A.

1994-01-01

Our work was primarily theoretical and numerical. We investigated the simplified modeling of heat losses in diffusion flames, then we 'ramped up' the level of complexity in each successive study until the final chapter discussed the general problem of soot/flame interaction. With regard to the specific objective of studying radiative extinction, we conclude that in the steady case a self-extinguishing zero-g flame is unlikely to occur. The soot volume fractions are too small. On the other hand, our work does provide rational means for assessing the mixture of chemical energy release and radiative heat release. It also provides clues for suitable 'tailoring' this balance. Thus heat fluxes to surrounding surfaces can be substantially increased by exploiting and modifying its sooting capability.

Recovery of a Charred Painting Using Atomic Oxygen Treatment

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Banks, Bruce A.; Chichernea, Virgil A.

1999-01-01

A noncontact method is described which uses atomic oxygen to remove soot and char from the surface of a painting. The atomic oxygen was generated by the dissociation of oxygen in low pressure air using radio frequency energy. The treatment, which is an oxidation process, allows control of the amount of material to be removed. The effectiveness of char removal from half of a fire-damaged oil painting was studied using reflected light measurements from selected areas of the painting and by visual and photographic observation. The atomic oxygen was able to effectively remove char and soot from the treated half of the painting. The remaining loosely bound pigment was lightly sprayed with a mist to replace the binder and then varnish was reapplied. Caution should he used when treating an untested paint medium using atomic oxygen. A representative edge or corner should he tested first in order to determine if the process would be safe for the pigments present. As more testing occurs, a greater knowledge base will be developed as to what types of paints and varnishes can or cannot be treated using this technique. With the proper precautions, atomic oxygen treatment does appear to be a technique with great potential for allowing very charred, previously unrestorable art to be salvaged.

Phototransformation rate constants of PAHs associated with soot particles.

PubMed

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

2013-01-15

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. Copyright © 2012 Elsevier B.V. All rights reserved.

Stronger association of polycyclic aromatic hydrocarbons with soot than with char in soils and sediments

PubMed Central

Han, Y.M.; Bandowe, B.A.M.; Wei, C.; Cao, J.J.; Wilcke, W.; Wang, G.H.; Ni, H.Y.; Jin, Z.D.; An, Z.S.; Yan, B.Z.

2016-01-01

The knowledge of the association of polycyclic aromatic hydrocarbons (PAHs) with organic matter and carbonaceous materials is critical for a better understanding of their environmental transport, fate, and toxicological effects. Extensive studies have been done with regard to the relationship of PAHs with total organic carbon (TOC) and elemental carbon (EC) in different environmental matrices. The relationship between PAHs and the two subtypes of EC, char (combustion residues) and soot (produced via gas-to-particle conversion) also has been tested in field and laboratory experiments using reference materials. However, a direct comparison of associations of PAHs between with char and with soot in real environmental matrices has to our knowledge not yet been reported because of a lack of methodology to differentiate them. In this study, char and soot were measured using the IMPROVE method to test their associations with 12 EPA priority PAHs measured in topsoil samples (N = 22, top 10 cm) collected from the Guanzhong Plain and in surface sediment samples (N = 32, top 5 cm) from the Wei River (central China). In both soils and sediments, Σ12PAHs were more strongly associated with soot than with char, mainly due to the fact that soot and PAHs were produced in the same gas phase during combustion, had a strong affinity for each other, and were transported and deposited together, while char, the combustion residue, was transported differently to PAHs due to its large particle size. Stronger correlations between PAHs and the different carbon fractions (TOC, soot, and char) in sediments than in soils were observed, which is associated with the redistribution of PAHs among the organic matter pools in water because of the processes during soil erosion and sedimentation in the river. PMID:24656973

Computational and experimental study of laminar flames

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smooke, Mitchell

During the past three years, our research has centered on an investigation of the effects of complex chemistry and detailed transport on the structure and extinction of hydrocarbon flames in coflowing axisymmetric configurations. We have pursued both computational and experimental aspects of the research in parallel on both steady-state and time-dependent systems. The computational work has focused on the application of accurate and efficient numerical methods for the solution of the steady-state and time-dependent boundary value problems describing the various reacting systems. Detailed experimental measurements were performed on axisymmetric coflow flames using two-dimensional imaging techniques. Previously, spontaneous Raman scattering, chemiluminescence,more » and laser-induced fluorescence were used to measure the temperature, major and minor species profiles. Particle image velocimetry (PIV) has been used to investigate velocity distributions and for calibration of time-varying flames. Laser-induced incandescence (LII) with an extinction calibration was used to determine soot volume fractions, while soot surface temperatures were measured with three-color optical pyrometry using a color digital camera. A blackbody calibration of the camera allows for determination of soot volume fraction as well, which can be compared with the LII measurements. More recently, we have concentrated on a detailed characterization of soot using a variety of techniques including time-resolved LII (TiRe-LII) for soot primary particles sizes, multi-angle light scattering (MALS) for soot radius of gyration, and spectrally-resolved line of sight attenuation (spec-LOSA). Combining the information from all of these soot measurements can be used to determine the soot optical properties, which are observed to vary significantly depending on spatial location and fuel dilution. Our goal has been to obtain a more fundamental understanding of the important fluid dynamic and chemical interactions in these flames so that this information can be used effectively in combustion modeling.« less

Flame Retardant Effect of Nano Fillers on Polydimethylsiloxane Composites.

PubMed

Jagdale, Pravin; Salimpour, Samera; Islam, Md Hujjatul; Cuttica, Fabio; Hernandez, Francisco C Robles; Tagliaferro, Alberto; Frache, Alberto

2018-02-01

Polydimethylsiloxane has exceptional fire retardancy characteristics, which make it a popular polymer in flame retardancy applications. Flame retardancy of polydimethylsiloxane with different nano fillers was studied. Polydimethylsiloxane composite fire property varies because of the shape, size, density, and chemical nature of nano fillers. In house made carbon and bismuth oxide nano fillers were used in polydimethylsiloxane composite. Carbon from biochar (carbonised bamboo) and a carbon by-product (carbon soot) were selected. For comparative study of nano fillers, standard commercial multiwall carbon nano tubes (functionalised, graphitised and pristine) as nano fillers were selected. Nano fillers in polydimethylsiloxane positively affects their fire retardant properties such as total smoke release, peak heat release rate, and time to ignition. Charring and surface ceramization are the main reasons for such improvement. Nano fillers in polydimethylsiloxane may affect the thermal mobility of polymer chains, which can directly affect the time to ignition. The study concludes that the addition of pristine multiwall carbon nano tubes and bismuth oxide nano particles as filler in polydimethylsiloxane composite improves the fire retardant property.

Impact of rail pressure and biodiesel fueling on the particulate morphology and soot nanostructures from a common-rail turbocharged direct injection diesel engine

DOE PAGES

Ye, Peng; Vander Wal, Randy; Boehman, Andre L.; ...

2014-12-26

The effect of rail pressure and biodiesel fueling on the morphology of exhaust particulate agglomerates and the nanostructure of primary particles (soot) was investigated with a common-rail turbocharged direct injection diesel engine. The engine was operated at steady state on a dynamometer running at moderate speed with both low (30%) and medium–high (60%) fixed loads, and exhaust particulate was sampled for analysis. Ultra-low sulfur diesel and its 20% v/v blends with soybean methyl ester biodiesel were used. Fuel injection occurred in a single event around top dead center at three different injection pressures. Exhaust particulate samples were characterized with TEMmore » imaging, scanning mobility particle sizing, thermogravimetric analysis, Raman spectroscopy, and XRD analysis. Particulate morphology and oxidative reactivity were found to vary significantly with rail pressure and with biodiesel blend level. Higher biodiesel content led to increases in the primary particle size and oxidative reactivity but did not affect nanoscale disorder in the as-received samples. For particulates generated with higher injection pressures, the initial oxidative reactivity increased, but there was no detectable correlation with primary particle size or nanoscale disorder.« less

Impact of rail pressure and biodiesel fueling on the particulate morphology and soot nanostructures from a common-rail turbocharged direct injection diesel engine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ye, Peng; Vander Wal, Randy; Boehman, Andre L.

The effect of rail pressure and biodiesel fueling on the morphology of exhaust particulate agglomerates and the nanostructure of primary particles (soot) was investigated with a common-rail turbocharged direct injection diesel engine. The engine was operated at steady state on a dynamometer running at moderate speed with both low (30%) and medium–high (60%) fixed loads, and exhaust particulate was sampled for analysis. Ultra-low sulfur diesel and its 20% v/v blends with soybean methyl ester biodiesel were used. Fuel injection occurred in a single event around top dead center at three different injection pressures. Exhaust particulate samples were characterized with TEMmore » imaging, scanning mobility particle sizing, thermogravimetric analysis, Raman spectroscopy, and XRD analysis. Particulate morphology and oxidative reactivity were found to vary significantly with rail pressure and with biodiesel blend level. Higher biodiesel content led to increases in the primary particle size and oxidative reactivity but did not affect nanoscale disorder in the as-received samples. For particulates generated with higher injection pressures, the initial oxidative reactivity increased, but there was no detectable correlation with primary particle size or nanoscale disorder.« less

Air pollution from aircraft

NASA Technical Reports Server (NTRS)

Heywood, J. B.; Fay, J. A.; Chigier, N. A.

1979-01-01

A series of fundamental problems related to jet engine air pollution and combustion were examined. These include soot formation and oxidation, nitric oxide and carbon monoxide emissions mechanisms, pollutant dispension, flow and combustion characteristics of the NASA swirl can combustor, fuel atomization and fuel-air mixing processes, fuel spray drop velocity and size measurement, ignition and blowout. A summary of this work, and a bibliography of 41 theses and publications which describe this work, with abstracts, is included.

Combustion Processes in Hybrid Rocket Engines

NASA Technical Reports Server (NTRS)

Venkateswaran,S.; Merkle, C. L.

1996-01-01

In recent years, there has been a resurgence of interest in the development of hybrid rocket engines for advanced launch vehicle applications. Hybrid propulsion systems use a solid fuel such as hydroxyl-terminated polybutadiene (HTPB) along with a gaseous/liquid oxidizer. The performance of hybrid combustors depends on the convective and radiative heat fluxes to the fuel surface, the rate of pyrolysis in the solid phase, and the turbulent combustion processes in the gaseous phases. These processes in combination specify the regression rates of the fuel surface and thereby the utilization efficiency of the fuel. In this paper, we employ computational fluid dynamics (CFD) techniques in order to gain a quantitative understanding of the physical trends in hybrid rocket combustors. The computational modeling is tailored to ongoing experiments at Penn State that employ a two dimensional slab burner configuration. The coordinated computational/experimental effort enables model validation while providing an understanding of the experimental observations. Computations to date have included the full length geometry with and with the aft nozzle section as well as shorter length domains for extensive parametric characterization. HTPB is sed as the fuel with 1,3 butadiene being taken as the gaseous product of the pyrolysis. Pure gaseous oxygen is taken as the oxidizer. The fuel regression rate is specified using an Arrhenius rate reaction, which the fuel surface temperature is given by an energy balance involving gas-phase convection and radiation as well as thermal conduction in the solid-phase. For the gas-phase combustion, a two step global reaction is used. The standard kappa - epsilon model is used for turbulence closure. Radiation is presently treated using a simple diffusion approximation which is valid for large optical path lengths, representative of radiation from soot particles. Computational results are obtained to determine the trends in the fuel burning or regression rates as a function of the head-end oxidizer mass flux, G=rho(e)U(e), and the chamber pressure. Furthermore, computation of the full slab burner configuration has also been obtained for various stages of the burn. Comparisons with available experimental data from small scale tests conducted by General Dynamics-Thiokol-Rocketdyne suggest reasonable agreement in the predicted regression rates. Future work will include: (1) a model for soot generation in the flame for more quantitative radiative transfer modelling, (2) a parametric study of combustion efficiency, and (3) transient calculations to help determine the possible mechanisms responsible for combustion instability in hybrid rocket motors.

Reconstruction model for temperature and concentration profiles of soot and metal-oxide nanoparticles in a nanofluid fuel flame by using a CCD camera

NASA Astrophysics Data System (ADS)

Liu, Guannan; Liu, Dong

2018-05-01

Not Available Project supported by the National Natural Science Foundation of China (Grant No. 51576100) and the Project of “Six Talent Summit” of Jiangsu Province, China (Grant No. 2014-XNY-002).

EFFECT OF SOOT, TEMPERATURE AND RESIDENCE TIME ON PCDD/F FORMATION

EPA Science Inventory

Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) are formed during thermal processes in the presence of fly ash that acts as an oxidation catalyst as well as a carbon and chloride source. Recent laboratory studies pointed out the importance of s...

Particulate matter from both heavy fuel oil and diesel fuel shipping emissions show strong biological effects on human lung cells at realistic and comparable in vitro exposure conditions.

PubMed

Oeder, Sebastian; Kanashova, Tamara; Sippula, Olli; Sapcariu, Sean C; Streibel, Thorsten; Arteaga-Salas, Jose Manuel; Passig, Johannes; Dilger, Marco; Paur, Hanns-Rudolf; Schlager, Christoph; Mülhopt, Sonja; Diabaté, Silvia; Weiss, Carsten; Stengel, Benjamin; Rabe, Rom; Harndorf, Horst; Torvela, Tiina; Jokiniemi, Jorma K; Hirvonen, Maija-Riitta; Schmidt-Weber, Carsten; Traidl-Hoffmann, Claudia; BéruBé, Kelly A; Wlodarczyk, Anna J; Prytherch, Zoë; Michalke, Bernhard; Krebs, Tobias; Prévôt, André S H; Kelbg, Michael; Tiggesbäumker, Josef; Karg, Erwin; Jakobi, Gert; Scholtes, Sorana; Schnelle-Kreis, Jürgen; Lintelmann, Jutta; Matuschek, Georg; Sklorz, Martin; Klingbeil, Sophie; Orasche, Jürgen; Richthammer, Patrick; Müller, Laarnie; Elsasser, Michael; Reda, Ahmed; Gröger, Thomas; Weggler, Benedikt; Schwemer, Theo; Czech, Hendryk; Rüger, Christopher P; Abbaszade, Gülcin; Radischat, Christian; Hiller, Karsten; Buters, Jeroen T M; Dittmar, Gunnar; Zimmermann, Ralf

2015-01-01

Ship engine emissions are important with regard to lung and cardiovascular diseases especially in coastal regions worldwide. Known cellular responses to combustion particles include oxidative stress and inflammatory signalling. To provide a molecular link between the chemical and physical characteristics of ship emission particles and the cellular responses they elicit and to identify potentially harmful fractions in shipping emission aerosols. Through an air-liquid interface exposure system, we exposed human lung cells under realistic in vitro conditions to exhaust fumes from a ship engine running on either common heavy fuel oil (HFO) or cleaner-burning diesel fuel (DF). Advanced chemical analyses of the exhaust aerosols were combined with transcriptional, proteomic and metabolomic profiling including isotope labelling methods to characterise the lung cell responses. The HFO emissions contained high concentrations of toxic compounds such as metals and polycyclic aromatic hydrocarbon, and were higher in particle mass. These compounds were lower in DF emissions, which in turn had higher concentrations of elemental carbon ("soot"). Common cellular reactions included cellular stress responses and endocytosis. Reactions to HFO emissions were dominated by oxidative stress and inflammatory responses, whereas DF emissions induced generally a broader biological response than HFO emissions and affected essential cellular pathways such as energy metabolism, protein synthesis, and chromatin modification. Despite a lower content of known toxic compounds, combustion particles from the clean shipping fuel DF influenced several essential pathways of lung cell metabolism more strongly than particles from the unrefined fuel HFO. This might be attributable to a higher soot content in DF. Thus the role of diesel soot, which is a known carcinogen in acute air pollution-induced health effects should be further investigated. For the use of HFO and DF we recommend a reduction of carbonaceous soot in the ship emissions by implementation of filtration devices.

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

NASA Astrophysics Data System (ADS)

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 Lüönd et al. (2010) and Murray et al. (2011). Heterogeneous ice nucleation rate coefficients are derived which can be used to describe the immersion freezing process size-segregated in cloud microphysical models.

Contribution of Tula Refinery flaring emissions to the Mexico megacity

NASA Astrophysics Data System (ADS)

Almanza, Victor; Molina, Luisa; Sosa, Gustavo

2013-04-01

Flaring is an important source of greenhouse gases, particulate matter and Volatile Organic Compounds (VOCs) in both upstream and downstream operations in the oil and gas industry. In 2010 Mexico was the eleventh emitting country with 2.5 billion cubic meters of gas flared (World Bank, 2012). Black carbon (a component of soot) emissions from flaring facilities are of particular interest because soot is considered a short-lived climate forcer (SLCF) (UNEP, 2011). In 2011 there were 23 megacities of at least 10 million inhabitants. It is expected that this number increase to 37 by 2025, which will include one more in Northern America (NA) and two more in Latin America (UN, 2012). International collaborative projects like MILAGRO in NA and MEGAPOLI/CityZen in Europe, have been conducted to assess the impact of megacities air pollution at several scales. The former focused on the air pollution plume of Mexico City Metropolitan Area (MCMA), the largest megacity in NA. This work studies the contribution of flaring emissions from Tula Refinery to regional air quality. This is accomplished in two steps. First, the flame of a representative sour gas flare is modeled with a CFD combustion code in order to estimate emission rates of combustion by-products of interest for air quality. Mass flow rates of acetylene, ethylene, nitrogen oxides, carbon monoxide, soot and sulfur dioxide are obtained. The emission rates of NO2 and SO2 are compared with measurements obtained at Tula as part of MILAGRO field campaign. The rates of soot, VOCs and CO emissions are compared with estimates obtained by Instituto Mexicano del Petróleo (IMP). The second stage takes the flaring emission rates of the aforementioned species as inputs to WRF-Chem in order to simulate the chemical transport of the plume from 22 March to 27 March of 2006. The air quality model presented reliable performance of the resolved meteorology, with respect to the Mean Absolute Error (MAE), Root Mean Square Error (RMSE), mean bias (BIAS), vector RMSE and Index of Agreement (IOA). WRF-Chem outputs of SO2 and soot are compared with surface measurements obtained at the three supersites of MILAGRO campaign. Results suggest a contribution of Tula flaring activities to the total SO2 levels at the urban supersite (T0) of 37 %, and of 39 % at the suburban supersite (T1). In the MCMA, modeled SO2 is compared with representative monitoring stations of the MCMA Monitoring Network (RAMA). The suggested contribution is about 43 % and 36 % at the north and south regions of the basin respectively. As for soot, results indicate low contribution at the three supersites, with less than 0.1% at three supersites. According to the model, the greatest contribution of Tula flaring emissions to the three supersites and the MCMA basin occurred on 23 March, which coincided with the third cold surge event reported during the campaign.

Combustion products of 1,3-butadiene inhibit catalase activity and induce expression of oxidative DNA damage repair enzymes in human bronchial epithelial cells.

PubMed

Kennedy, Christopher H; Catallo, W James; Wilson, Vincent L; Mitchell, James B

2009-10-01

1,3-Butadiene, an important petrochemical, is commonly burned off when excess amounts need to be destroyed. This combustion process produces butadiene soot (BDS), which is composed of a complex mixture of polycyclic aromatic hydrocarbons in particulates ranging in size from <1 microm to 1 mm. An organic extract of BDS is both cytotoxic and genotoxic to normal human bronchial epithelial (NHBE) cells. Based on the oxidizing potential of BDS, we hypothesized that an organic extract of this particulate matter would (1) cause enzyme inactivation due to protein amino acid oxidation and (2) induce oxidative DNA damage in NHBE cells. Thus, our aims were to determine the effect of butadiene soot ethanol extract (BSEE) on both enzyme activity and the expression of proteins involved in the repair of oxidative DNA damage. Catalase was found to be sensitive to BDS as catalase activity was potently diminished in the presence of BSEE. Using Western analysis, both the alpha isoform of human 8-oxoguanine DNA glycosylase (alpha-hOGG1) and human apurinic/apyrimidinic endonuclease (APE-1) were shown to be significantly overexpressed as compared to untreated controls after exposure of NHBE cells to BSEE. Our results indicate that BSEE is capable of effectively inactivating the antioxidant enzyme catalase, presumably via oxidation of protein amino acids. The presence of oxidized biomolecules may partially explain the extranuclear fluorescence that is detected when NHBE cells are treated with an organic extract of BDS. Overexpression of both alpha-hOGG1 and APE-1 proteins following treatment of NHBE cells with BSEE suggests that this mixture causes oxidative DNA damage.

Combustion products of 1,3-butadiene inhibit catalase activity and induce expression of oxidative DNA damage repair enzymes in human bronchial epithelial cells

PubMed Central

Kennedy, Christopher H.; Catallo, W. James; Wilson, Vincent L.; Mitchell, James B.

2012-01-01

1,3-Butadiene, an important petrochemical, is commonly burned off when excess amounts need to be destroyed. This combustion process produces butadiene soot (BDS), which is composed of a complex mixture of polyaromatic hydrocarbons in particulates ranging in size from <1μm to 1 mm. An organic extract of BDS is both cytotoxic and genotoxic to normal human bronchial epithelial (NHBE) cells. Based on the oxidizing potential of BDS, we hypothesized that an organic extract of this particulate matter would: 1) cause enzyme inactivation due to protein amino acid oxidation; and 2) induce oxidative DNA damage in NHBE cells. Thus, our aims were to determine the effect of butadiene soot ethanol extract (BSEE) on both enzyme activity and expression of proteins involved in the repair of oxidative DNA damage. Catalase was found to be sensitive to BDS as catalase activity was potently diminished in the presence of BSEE. Using Western analysis, both the alpha isoform of human 8-oxoguanine DNA glycosylase (α-hOGG1) and human apurinic/apyrimidinic endonuclease (APE-1) were shown to be significantly overexpressed as compared to untreated controls after exposure of NHBE cells to BSEE. Our results indicate that BSEE is capable of effectively inactivating the antioxidant enzyme catalase, presumably via oxidation of protein amino acids. The presence of oxidized proteins may partially explain the extranuclear fluorescence that is detected when NHBE cells are treated with an organic extract of BDS. Overexpression of both α-hOGG1 and APE-1 proteins following treatment of NHBE cells with BSEE suggests that this mixture causes oxidative DNA damage. PMID:18685817

Plasma regenerated particulate trap and NO.sub.x reduction system

DOEpatents

Penetrante, Bernardino M.; Vogtlin, George E.; Merritt, Bernard T.; Brusasco, Raymond M.

2000-01-01

A non-catalytic two-stage process for removal of NO.sub.x and particulates from engine exhaust comprises a first stage that plasma converts NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons, and a second stage, which preferably occurs simultaneously with the first stage, that converts NO.sub.2 and carbon soot particles to respective environmentally benign gases that include N.sub.2 and CO.sub.2. By preconverting NO to NO.sub.2 in the first stage, the efficiency of the second stage for NO.sub.x reduction is enhanced while carbon soot from trapped particulates is simultaneously converted to CO.sub.2 when reacting with the NO.sub.2 (that converts to N.sub.2). For example, an internal combustion engine exhaust is connected by a pipe to a chamber where carbon-containing particulates are electrostatically trapped or filtered and a non-thermal plasma converts NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons. Volatile hydrocarbons (C.sub.x H.sub.y) from the trapped particulates are oxidized in the plasma and the remaining soot from the particulates reacts with the NO.sub.2 to convert NO.sub.2 to N.sub.2, and the soot to CO.sub.2. The nitrogen exhaust components remain in the gas phase throughout the process, with no accompanying adsorption.

Internally mixed sea salt, soot, and sulfates at Macao, a coastal city in South China.

PubMed

Li, Weijun; Shao, Longyi; Shen, Rongrong; Yang, Shusheng; Wang, Zhishi; Tang, Uwa

2011-11-01

Direct observation of the mixing state of aerosol particles in a coastal urban city is critical to understand atmospheric processing and hygroscopic growth in humid air. Morphology, composition, and mixing state of individual aerosol particles from Macao, located south of the Pearl River Delta (PRD) and 100 km west of Hong Kong, were investigated using scanning electron microscopy (SEM) and transmission electron microscopy coupled with energy-dispersive X-ray spectrometry (TEM/EDX). SEM images show that soot and roughly spherical particles are prevalent in the samples. Based on the compositions of individual aerosol particles, aerosol particles with roughly spherical shape are classified into coarse Na-rich and fine S-rich particles. TEM/EDX indicates that each Na-rich particle consists of a Na-S core and NaNO3 shell. Even in the absence of heavy pollution, the marine sea salt particles were completely depleted in chloride, and Na-related sulfates and nitrates were enriched in Macao air. The reason could be that SO2 from the polluted PRD and ships in the South China Sea and NO2 from vehicles in the city sped up the chlorine depletion in sea salt through heterogeneous reactions. Fresh soot particles from vehicular emissions mainly occur near curbside. However, there are many aged soot particles in the sampling site surrounded by main roads 200 to 400 m away, suggesting that the fresh soot likely underwent a quick aging. Overall, secondary nitrates and sulfates internally mixed with soot and sea salt particles can totally change their surface hygroscopicity in coastal cities.

Shapes of Soot Particles Embedded in Organic Material and Sulfates

NASA Astrophysics Data System (ADS)

Adachi, K.; Buseck, P. R.

2008-12-01

Three-dimensional (3D) shapes of aerosol particles collected from Mexico City during the MILAGRO (Megacity Initiative: Local and Global Research Observations) campaign were analyzed using electron tomography (ET). Mexico City is a representative tropical megacity, where pollution is heavy and photochemical reaction is rapid. Its aerosol particles are of interest because of their effects on the regional and global climate and on health. We used ET to study soot particles that are embedded in organic material, commonly with sulfates, collected from Mexico City plumes. They comprise more than 50 % of the aerosol particles with aerodynamic diameters between 50 and 300 nm. ET combines a series of transmission electron microscope (TEM) images obtained in different viewing directions into representations that display the 3D digitized objects. By using the 3D data, we determined the volume ratios of the various component materials in individual internally mixed particles. In our samples, organic materials dominate, and soot and sulfate commonly occupy up to 10 volume %. The mean fractal dimension, which indicates the complexity of aggregates, of soot particles is 2.2 (± 0.2), suggesting that they retain their chain-like structure when embedded in organic material rather than being highly compacted. Their 3D images show that soot particles tend to be near the surface of the embedding particle rather than in the core, i.e., a core-shell model is inappropriate. Their morphological features indicate that the soot particles have lower absorption of sunlight by a few tens of percent relative to that of the compacted or concentrically coated particles assumed in current climate models.

Climate and chemistry effects of a regional scale nuclear conflict

NASA Astrophysics Data System (ADS)

Stenke, A.; Hoyle, C. R.; Luo, B.; Rozanov, E.; Gröbner, J.; Maag, L.; Brönnimann, S.; Peter, T.

2013-05-01

Previous studies have highlighted the severity of detrimental effects for life on Earth after an assumed regionally limited nuclear war. These effects are caused by climatic, chemical and radiative changes persisting for up to one decade. However, so far only a very limited number of climate model simulations have been performed, giving rise to the question how realistic previous computations have been. This study uses the coupled chemistry climate model (CCM) SOCOL, which belongs to a different family of CCMs than previously used, to investigate the consequences of such a hypothetical nuclear conflict. In accordance with previous studies, the present work assumes a scenario of a nuclear conflict between India and Pakistan, each applying 50 warheads with an individual blasting power of 15 kt ("Hiroshima size") against the major population centers, resulting in the emission of tiny soot particles, which are generated in the firestorms expected in the aftermath of the detonations. Substantial uncertainties related to the calculation of likely soot emissions, particularly concerning assumptions of target fuel loading and targeting of weapons, have been addressed by simulating several scenarios, with soot emissions ranging from 1 to 12 Tg. Their high absorptivity with respect to solar radiation leads to a tremendous self-lofting of the soot particles into the strato- and mesosphere, where they remain for several years. Consequently, the model suggests Earth's surface temperatures to drop by several degrees Celsius due to the shielding of solar irradiance by the soot, indicating a major global cooling. In addition, there is a substantial reduction of precipitation lasting 5 to 10 yr after the conflict, depending on the magnitude of the initial soot release. Extreme cold spells associated with massive sea ice formation are found during Northern Hemisphere winter, which expose the continental land masses of Northern America and Eurasia to chilling coldness. In the stratosphere, the strong heating leads to an acceleration of catalytic ozone loss and, consequently, to enhancements of UV radiation at the ground. In contrast to surface temperature and precipitation changes, which show a linear dependence to the soot burden, there is a saturation effect with respect to stratospheric ozone chemistry. Soot emissions of 5 Tg lead to an ozone column reduction of almost 50% in northern high latitudes, while emitting 12 Tg only increases ozone loss by a further 10%. In summary, this study, though using a different chemistry climate model, corroborates the previous investigations with respect to the atmospheric impacts. In addition to these persistent effects, the present study draws attention to episodically cold phases, which would likely add to the severity of human harm worldwide. The best insurance against such a catastrophic development would be the delegitimization of nuclear weapons.

Climate and chemistry effects of a regional scale nuclear conflict

NASA Astrophysics Data System (ADS)

Stenke, A.; Hoyle, C. R.; Luo, B.; Rozanov, E.; Gröbner, J.; Maag, L.; Brönnimann, S.; Peter, T.

2013-10-01

Previous studies have highlighted the severity of detrimental effects for life on earth after an assumed regionally limited nuclear war. These effects are caused by climatic, chemical and radiative changes persisting for up to one decade. However, so far only a very limited number of climate model simulations have been performed, giving rise to the question how realistic previous computations have been. This study uses the coupled chemistry climate model (CCM) SOCOL, which belongs to a different family of CCMs than previously used, to investigate the consequences of such a hypothetical nuclear conflict. In accordance with previous studies, the present work assumes a scenario of a nuclear conflict between India and Pakistan, each applying 50 warheads with an individual blasting power of 15 kt ("Hiroshima size") against the major population centers, resulting in the emission of tiny soot particles, which are generated in the firestorms expected in the aftermath of the detonations. Substantial uncertainties related to the calculation of likely soot emissions, particularly concerning assumptions of target fuel loading and targeting of weapons, have been addressed by simulating several scenarios, with soot emissions ranging from 1 to 12 Tg. Their high absorptivity with respect to solar radiation leads to a rapid self-lofting of the soot particles into the strato- and mesosphere within a few days after emission, where they remain for several years. Consequently, the model suggests earth's surface temperatures to drop by several degrees Celsius due to the shielding of solar irradiance by the soot, indicating a major global cooling. In addition, there is a substantial reduction of precipitation lasting 5 to 10 yr after the conflict, depending on the magnitude of the initial soot release. Extreme cold spells associated with an increase in sea ice formation are found during Northern Hemisphere winter, which expose the continental land masses of North America and Eurasia to a cooling of several degrees. In the stratosphere, the strong heating leads to an acceleration of catalytic ozone loss and, consequently, to enhancements of UV radiation at the ground. In contrast to surface temperature and precipitation changes, which show a linear dependence to the soot burden, there is a saturation effect with respect to stratospheric ozone chemistry. Soot emissions of 5 Tg lead to an ozone column reduction of almost 50% in northern high latitudes, while emitting 12 Tg only increases ozone loss by a further 10%. In summary, this study, though using a different chemistry climate model, corroborates the previous investigations with respect to the atmospheric impacts. In addition to these persistent effects, the present study draws attention to episodically cold phases, which would likely add to the severity of human harm worldwide. The best insurance against such a catastrophic development would be the delegitimization of nuclear weapons.

Interaction between Air Bubbles and Superhydrophobic Surfaces in Aqueous Solutions.

PubMed

Shi, Chen; Cui, Xin; Zhang, Xurui; Tchoukov, Plamen; Liu, Qingxia; Encinas, Noemi; Paven, Maxime; Geyer, Florian; Vollmer, Doris; Xu, Zhenghe; Butt, Hans-Jürgen; Zeng, Hongbo

2015-07-07

Superhydrophobic surfaces are usually characterized by a high apparent contact angle of water drops in air. Here we analyze the inverse situation: Rather than focusing on water repellency in air, we measure the attractive interaction of air bubbles and superhydrophobic surfaces in water. Forces were measured between microbubbles with radii R of 40-90 μm attached to an atomic force microscope cantilever and submerged superhydrophobic surfaces. In addition, forces between macroscopic bubbles (R = 1.2 mm) at the end of capillaries and superhydrophobic surfaces were measured. As superhydrophobic surfaces we applied soot-templated surfaces, nanofilament surfaces, micropillar arrays with flat top faces, and decorated micropillars. Depending on the specific structure of the superhydrophobic surfaces and the presence and amount of entrapped air, different interactions were observed. Soot-templated surfaces in the Cassie state showed superaerophilic behavior: Once the electrostatic double-layer force and a hydrodynamic repulsion were overcome, bubbles jumped onto the surface and fully merged with the entrapped air. On nanofilaments and micropillar arrays we observed in addition the formation of sessile bubbles with finite contact angles below 90° or the attachment of bubbles, which retained their spherical shape.

Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

PubMed

Canagaratna, Manjula R; Massoli, Paola; Browne, Eleanor C; Franklin, Jonathan P; Wilson, Kevin R; Onasch, Timothy B; Kirchstetter, Thomas W; Fortner, Edward C; Kolb, Charles E; Jayne, John T; Kroll, Jesse H; Worsnop, Douglas R

2015-05-14

Black carbon is an important constituent of atmospheric aerosol particle matter (PM) with significant effects on the global radiation budget and on human health. The soot particle aerosol mass spectrometer (SP-AMS) has been developed and deployed for real-time ambient measurements of refractory carbon particles. In the SP-AMS, black carbon or metallic particles are vaporized through absorption of 1064 nm light from a CW Nd:YAG laser. This scheme allows for continuous "soft" vaporization of both core and coating materials. The main focus of this work is to characterize the extent to which this vaporization scheme provides enhanced chemical composition information about aerosol particles. This information is difficult to extract from standard SP-AMS mass spectra because they are complicated by extensive fragmentation from the harsh 70 eV EI ionization scheme that is typically used in these instruments. Thus, in this work synchotron-generated vacuum ultraviolet (VUV) light in the 8-14 eV range is used to measure VUV-SP-AMS spectra with minimal fragmentation. VUV-SP-AMS spectra of commercially available carbon black, fullerene black, and laboratory generated flame soots were obtained. Small carbon cluster cations (C(+)-C5(+)) were found to dominate the VUV-SP-AMS spectra of all the samples, indicating that the corresponding neutral clusters are key products of the SP vaporization process. Intercomparisons of carbon cluster ratios observed in VUV-SP-AMS and SP-AMS spectra are used to confirm spectral features that could be used to distinguish between different types of refractory carbon particles. VUV-SP-AMS spectra of oxidized organic species adsorbed on absorbing cores are also examined and found to display less thermally induced decomposition and fragmentation than spectra obtained with thermal vaporization at 200 °C (the minimum temperature needed to quantitatively vaporize ambient oxidized organic aerosol with a continuously heated surface). The particle cores tested in these studies include black carbon, silver, gold, and platinum nanoparticles. These results demonstrate that SP vaporization is capable of providing enhanced organic chemical composition information for a wide range of organic coating materials and IR absorbing particle cores. The potential of using this technique to study organic species of interest in seeded laboratory chamber or flow reactor studies is discussed.

Boundary Layer Study. Experimental Validation Test Plan. Phase 4

DTIC Science & Technology

1990-11-01

34 Ph.D. Thesis. 2. "The Importance of Soot Particles and Nitrous Acid in Oxidizing 802 in Atmospheric Aqueous Droplets," with S.G. Chang and T. Novakov ...4. "Lifetime of Aerosol Droplets in Ambient Air: Consideration of the Effects of Surfactants and Chemical Reaction," with T. Novakov Atmgsoheric...California, 1975. 6. "Sulfur Dioxide Oxidation in a Dispersing Plumse," with S.G. Chang and T. Novakov , Atmosnherlic Aerosol Research Annual Report

Electron spin resonance of particulate soot samples from automobiles to help environmental studies.

PubMed

Yamanaka, C; Matsuda, T; Ikeya, M

2005-02-01

The application of electron spin resonance (ESR) was studied for diesel soot samples and suspended particulate matter (SPM) from automobile engines. Soot samples or diesel exhaust particles (DEP) were recovered at various points: in the exhaust pipe of a diesel engine, at the dust sampler of a highway tunnel (standard DEP), on the soundproofing wall alongside a heavy traffic road, and on the filters of a dust sampler for SPM. The diesel soot samples apparently showed two ESR spectra: one was a broad spectrum at g=2.1 with a line width of ca. 80-120 mT and the other was a sharp signal of a carbon radical at g=2.003 with a line width of 0.4 mT. Annealing experiments with a DEP sample at 250 degrees C revealed drastic enhancement of the sharp ESR signal, which suggested a thermal process of carbonization of remnant organics. An oximetric study by ESR showed an enhancement of the broad signal in the diesel soot sample as well as in the sharp ESR signal. Therefore, the main part of the broad ESR signal would be attributed to carbon radicals, which form a different configuration, probably closely interacting aggregates. Enhancement of the sharp ESR signal was not observed in the standard DEP sample under vacuum condition, which suggested less adsorption sites on the surface of DEP samples.

Treatment and Analysis of a Paint Chip from "Water Lilies": A Fire Damaged Monet

NASA Technical Reports Server (NTRS)

Miller, Sharon K. R.; Banks, Bruce A.; Tollis, Greg

2001-01-01

A museum fire in 1958 severely damaged a Monet 'Water Lilies' (1916-1926) painting that was on display. The surface of the painting is very dark with areas of blistering and charring. Over the years, traditional techniques have been found to be ineffective at removal of the soot and char from the surface. The painting, which is now in the care of the New York University (NYU) Conservation Center of the Institute of Fine Arts, was the subject of a study to determine if atomic oxygen treatment could remove the soot and char without damaging the fragile painting underneath. For test purposes, a small chip of paint was removed from the edge of the painting by a conservator at NYU and supplied to NASA Glenn Research Center for atomic oxygen treatment and analysis. The diffuse spectral reflectance, at three locations on the paint chip, was monitored at intervals during the atomic oxygen treatment process. Photo documentation of the chip during treatment was also performed. The color contrast was calculated from the spectral reflectance data as a function of treatment duration. Results of the testing indicated that the contrast improved as a result of the treatment, and the differentiation of colors on the surface was significantly improved. Soot and char could be removed without visibly affecting the gross surface features such as impasto areas. These results indicate the feasibility for the treatment of the 'Water Lilies' painting.

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

NASA Technical Reports Server (NTRS)

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 absence of asymmetrical forced and natural convection, a soot shell is formed between the droplet surface and the flame, exerting an influence on the droplet combustion response far greater than previously recognized. The effects of soot on droplet burning parameters, including burning rate, soot shell dynamics, flame structure, and extinction phenomena provide significant testing parameters for studying the structure and coupling of soot models with other sub-model components.

The surface chemical reactivity of particles and its impact on human health

NASA Astrophysics Data System (ADS)

Setyan, A.; Sauvain, J. J.; Riediker, M.; Guillemin, M.; Rossi, M. J.

2017-12-01

The chemical composition of the particle-air interface is the gateway to chemical reactions of gases with condensed phase particles. It is of prime importance to understand the reactivity of particles and their interaction with surrounding gases, biological membranes, and solid supports. We used a Knudsen flow reactor to quantify functional groups on the surface of a few selected particle types. This technique is based on a heterogeneous titration reaction between a probe gas and a specific functional group on the particle surface. Six probe gases have been selected for the identification and quantification of important functional groups: N(CH3)3 for the titration of acidic sites, NH2OH for the detection of carbonyl functions (aldehydes and ketones) and/or oxidized sites owing to its strong reducing properties, CF3COOH and HCl for basic sites of different strength, O3 and NO2 for oxidizable groups. We also studied the kinetics of the reactions between particles and probe gases (uptake coefficient γ0). We tested the surface chemical composition and oxidation states of laboratory-generated aerosols (3 amorphous carbons, 2 flame soots, 2 Diesel particles, 2 secondary organic aerosols [SOA], 4 multiwall carbon nanotubes [MWCNT], 3 TiO2, and 2 metal salts) and of aerosols sampled in several bus depots. The sampling of particles in the bus depots was accompanied by the collection of urine samples of mechanics working full-time in these bus depots, and the quantification of 8-hydroxy-2'-deoxyguanosine, a biomarker of oxidative stress. The increase in oxidative stress biomarker levels over a working day was correlated (p<0.05) with the number of olefinic and/or PAH sites on the surface of particles sampled at the bus depots, obtained from O3 uptakes, as well as with the initial uptake coefficient (γ0) of five probe gases used in the field. This correlation with γ0 suggests the idea of competing pathways occurring at the interface of the aerosol particles between the generation of reactive oxygen species (ROS) responsible for oxidative stress and cellular antioxidants.

Soot and Sulfuric Acid from Aircraft: Is There Enough to Cause Detrimental Environmental E-kCTSs?

NASA Technical Reports Server (NTRS)

Pueschel, R. F.; Strawa, A. W.; Ferry, G. V.; Howard, S. D.; Verma, S.

1998-01-01

Aerosol from aircraft can affect the environment in three ways: First, soot aerosol has been implicated to cause Icing-tern ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. 5% per decade. This effect is in addition and unrelated to the polar ozone holes which are strongly influenced by heterogeneous chemistry on polar stratospheric clouds. Second, the most obvious effect of jet aircraft is the formation of visible contrails in the upper troposphere. The Salt Lake City region experienced an 8% increase in cirrus cloud cover over a 15-year period which covariates with an increase in regional commercial air traffic. If soot particles act as freezing nuclei to cause contrail formation heterogeneously, they would be linked to a secondary effect to cloud modification that very likely is climatologically important. Third, a buildup of soot aerosol could reduce the single scatter albedo of stratospheric aerosol from 0.993+0.004 to 0.98, a critical value that has been postulated to separate stratospheric cooling from warming. Thus arises an important question: Do aircraft emit sufficient amounts of soot to have detrimental effects and warrant emission controls? During the 1996 SUCCESS field campaign, we sampled aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EI(sub H2SO4) = 9.0E-2 and 5.0E-1 g/kg (sub FUEL) for 75 and 675 ppm fuel-sulfur, respectively) and soot aerosol (2.2E-3 less than EI(sub SOOT) = l.lE-2 g/kg (sub FUEL)). The soot particle analysis accounted for their fractal nature, determined electron-microscopically, which enhanced the surface area by a factor of 26 and the volume 11-fold over equivalent-volume spheres. The corresponding fuel-sulfur to H2SO4 conversion efficiency was 10% (for 675 ppmm fuel-S) and 37% (for 75 ppmm fuel-S). Applying the H2SO4 emission index to the 1990 fuel use by the worlds commercial fleets of 1.3E11 kg, a conversion efficiency of 30% of 500 ppmm fuel-S would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4. This is about one part in 1.E4 of anthropogenic sulfate from other sources. The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E6 kg. Thus, soot amounts to only five percent of the aerosol generated by aircraft. Its reactivity with ozone would have to be 20 times that of sulfuric acid particles to make it chemically significant. Nevertheless, the findings, of stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II satellite extinction, against the "noise" due to volcanic eruptions. Observation of soot particles at 20 km altitude which, if emitted by aircraft were generated at 10-12 km altitude, suggests a displacement of those particles against gravity. Because eddy mixing is virtually absent in the lower stratosphere and isentropic mixing explains lofting to only about 15 km, radiometric forces acting on morphologically and chemically asymmetric soot particles must be considered a possibility. The consequence could be an extended residence time of soot against that of sulfuric acid aerosol that would lower the single scatter albedo with time.

Fragmentation and bond strength of airborne diesel soot agglomerates

PubMed Central

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

Morphology and Chemical Composition of soot particles emitted by Wood-burning Cook-Stoves: a HRTEM, XPS and Elastic backscattering Studies.

NASA Astrophysics Data System (ADS)

Carabali-Sandoval, G. A., Sr.; Castro, T.; Peralta, O.; De la Cruz, W.; Días, J.; Amelines, O.; Rivera-Hernández, M.; Varela, A.; Muñoz-Muñoz, F.; Policroniades, R.; Murillo, G.; Moreno, E.

2014-12-01

The morphology, microstructure and the chemical composition on surface of soot particles were studied by using high resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and elastic backscattering spectrometry. In order to obtain freshly soot particles emitted by home-made wood-burning cook stoves, copper grids for Transmission Electron Microscope (TEM) were placed on the last two of an 8-stages MOUDI cascade impactor. The analysis of HRTEM micrographs revealed the nanostructure and the particle size of soot particles. The XPS survey spectra show a large carbon peak around 285 eV and the oxygen signal at 533 eV. Some differences observed in the carbon/oxygen (C/O) ratio of the particles probably depend on the combustion process efficiency of each cook-stove analyzed. The C-1s XPS spectra show an asymmetric broad peak and other with low intensity that corresponds to sp2 and sp3hybridization, which were fitted with a convolution using Gaussian functions. Elastic backscattering technique allows a chemical elemental analysis of samples and confirms the presence of C, O and Si observed by XPS. Additionally, the morphological properties of soot aggregates were analyzed calculating the border-based fractal dimension (Df). Particles exhibit complex shapes with high values of Df. Also, real-time absorption (σabs) and scattering (σsct) coefficients of fine (with aerodynamic diameter < 2.5 µm) soot particles were measured. The trend in σabs and σsct indicate that the cooking process has two important combustion stages which varied in its flaming strength, being vigorous in the first stage and soft in the second one.

Understanding the Role of a nano Ce Additive in the Size Distribution and Organic Composition of Diesel Emissions

EPA Science Inventory

A number of alkali, alkaline earth, transition, and metalloid elements are known to act as fuel catalysts to limit the formation of soot precursors or promote its oxidation. These have been used with varying success on a variety of stationary and mobile combustion sources. Iron...

Kinetic Modeling of Polychlorinated Dibenzo-p-dioxin and Dibenzofuran Formation Based on Carbon Degradation Reactions

EPA Science Inventory

Combustion experiments in a laboratory-scale fixed bed reactor were performed to determine the role of temperature and time in PCDD/F formation allowing a global kinetic expression to be written for PCDD/F formation due to soot oxidation in fly ash deposits. Rate constants were c...

77 FR 34149 - Heavy-Duty Highway Program: Revisions for Emergency Vehicles and SCR Maintenance

Federal Register 2010, 2011, 2012, 2013, 2014

2012-06-08

... soot. Since this burning can involve extra heat and/or oxygen or oxygen- containing compounds, this... fuel consumption. This loss in performance may be noticed by the vehicle operator in terms of poor... excessive amounts of trapped PM begin to oxidize at high temperatures (i.e., DPF regeneration temperatures...

Nanotechnology and the Environment: Report of a National Nanotechnology Initiative Workshop Held in Arlington, Virginia on 8-9 May 2003

DTIC Science & Technology

2007-01-01

cover: Image shows an artist’s rendition of the core-shell structure of metal- oxide -coated palladium- doped zero-valent iron nanoparticles for catalytic...demonstrated the creation of functionalized gold nanoparticles (see figure c) without the need for many of the toxic solvents (e.g., diborane...Size-selected nanoparticle chemistry: Kinetics of soot oxidation , J. Phys. Chem. A 106, 96–103 (2002). 6. H. J. Tobias, D. E. Beving, P. J. Ziemann, H

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chianelli, Russell R.; Castillo, Karina; Gupta, Vipin

Photovoltaic devices and methods of making the same, are disclosed herein. The cell comprises a photovoltaic device that comprises a first electrically conductive layer comprising a photo-sensitized electrode; at least one photoelectrochemical layer comprising metal-oxide particles, an electrolyte solution comprising at least one asphaltene fraction, wherein the metal-oxide particles are optionally dispersed in a surfactant; and a second electrically conductive layer comprising a counter-electrode, wherein the second electrically conductive layer comprises one or more conductive elements comprising carbon, graphite, soot, carbon allotropes or any combinations thereof.

Formation and emission of large furans and oxygenated hydrocarbons from flames

PubMed Central

Johansson, K. Olof; Dillstrom, Tyler; Monti, Matteo; El Gabaly, Farid; Campbell, Matthew F.; Schrader, Paul E.; Popolan-Vaida, Denisia M.; Richards-Henderson, Nicole K.; Wilson, Kevin R.; Violi, Angela; Michelsen, Hope A.

2016-01-01

Many oxygenated hydrocarbon species formed during combustion, such as furans, are highly toxic and detrimental to human health and the environment. These species may also increase the hygroscopicity of soot and strongly influence the effects of soot on regional and global climate. However, large furans and associated oxygenated species have not previously been observed in flames, and their formation mechanism and interplay with polycyclic aromatic hydrocarbons (PAHs) are poorly understood. We report on a synergistic computational and experimental effort that elucidates the formation of oxygen-embedded compounds, such as furans and other oxygenated hydrocarbons, during the combustion of hydrocarbon fuels. We used ab initio and probabilistic computational techniques to identify low-barrier reaction mechanisms for the formation of large furans and other oxygenated hydrocarbons. We used vacuum-UV photoionization aerosol mass spectrometry and X-ray photoelectron spectroscopy to confirm these predictions. We show that furans are produced in the high-temperature regions of hydrocarbon flames, where they remarkably survive and become the main functional group of oxygenates that incorporate into incipient soot. In controlled flame studies, we discovered ∼100 oxygenated species previously unaccounted for. We found that large alcohols and enols act as precursors to furans, leading to incorporation of oxygen into the carbon skeletons of PAHs. Our results depart dramatically from the crude chemistry of carbon- and oxygen-containing molecules previously considered in hydrocarbon formation and oxidation models and spearhead the emerging understanding of the oxidation chemistry that is critical, for example, to control emissions of toxic and carcinogenic combustion by-products, which also greatly affect global warming. PMID:27410045

Formation and emission of large furans and oxygenated hydrocarbons from flames.

PubMed

Johansson, K Olof; Dillstrom, Tyler; Monti, Matteo; El Gabaly, Farid; Campbell, Matthew F; Schrader, Paul E; Popolan-Vaida, Denisia M; Richards-Henderson, Nicole K; Wilson, Kevin R; Violi, Angela; Michelsen, Hope A

2016-07-26

Many oxygenated hydrocarbon species formed during combustion, such as furans, are highly toxic and detrimental to human health and the environment. These species may also increase the hygroscopicity of soot and strongly influence the effects of soot on regional and global climate. However, large furans and associated oxygenated species have not previously been observed in flames, and their formation mechanism and interplay with polycyclic aromatic hydrocarbons (PAHs) are poorly understood. We report on a synergistic computational and experimental effort that elucidates the formation of oxygen-embedded compounds, such as furans and other oxygenated hydrocarbons, during the combustion of hydrocarbon fuels. We used ab initio and probabilistic computational techniques to identify low-barrier reaction mechanisms for the formation of large furans and other oxygenated hydrocarbons. We used vacuum-UV photoionization aerosol mass spectrometry and X-ray photoelectron spectroscopy to confirm these predictions. We show that furans are produced in the high-temperature regions of hydrocarbon flames, where they remarkably survive and become the main functional group of oxygenates that incorporate into incipient soot. In controlled flame studies, we discovered ∼100 oxygenated species previously unaccounted for. We found that large alcohols and enols act as precursors to furans, leading to incorporation of oxygen into the carbon skeletons of PAHs. Our results depart dramatically from the crude chemistry of carbon- and oxygen-containing molecules previously considered in hydrocarbon formation and oxidation models and spearhead the emerging understanding of the oxidation chemistry that is critical, for example, to control emissions of toxic and carcinogenic combustion by-products, which also greatly affect global warming.

Formation and emission of large furans and oxygenated hydrocarbons from flames

DOE PAGES

Johansson, K. Olof; Dillstrom, Tyler; Monti, Matteo; ...

2016-07-07

Many oxygenated hydrocarbon species formed during combustion, such as furans, are highly toxic and detrimental to human health and the environment. These species may also increase the hygroscopicity of soot and strongly influence the effects of soot on regional and global climate. However, large furans and associated oxygenated species have not previously been observed in flames, and their formation mechanism and interplay with polycyclic aromatic hydrocarbons (PAHs) are poorly understood. We report on a synergistic computational and experimental effort that elucidates the formation of oxygen-embedded compounds, such as furans and other oxygenated hydrocarbons, during the combustion of hydrocarbon fuels. Wemore » used ab initio and probabilistic computational techniques to identify low-barrier reaction mechanisms for the formation of large furans and other oxygenated hydrocarbons. We used vacuum-UV photoionization aerosol mass spectrometry and X-ray photoelectron spectroscopy to confirm these predictions. We show that fura ns are produced in the high- Temperature regions of hydrocarbon flames, where they remarkably survive and become the main functional group of oxygenates that incorporate into incipient soot. In controlled flame studies, we discovered ~100 oxygenated species previously unaccounted for. We found that large alcohols and enols act as precursors to furans, leading to incorporation of oxygen into the carbon skeletons of PAHs. Our results depart dramatically from the crude chemistry of carbonand oxygen-containing molecules previously considered in hydrocarbon formation and oxidation models and spearhead the emerging understanding of the oxidation chemistry that is critical, for example, to control emissions of toxic and carcinogenic combustion by-products, which also greatly affect global warming.« less

Effect of A-site deficiency in LaMn{sub 0.9}Co{sub 0.1}O{sub 3} perovskites on their catalytic performance for soot combustion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dinamarca, Robinson; Garcia, Ximena; Jimenez, Romel

Highlights: • A-site defective perovskites increases the oxidation state of the B-cation. • Not always non-stoichiometric perovskites exhibit higher catalytic activity in soot combustion. • The highly symmetric cubic crystalline structure diminishes the redox properties of perovskites. - Abstract: The influence of lanthanum stoichiometry in Ag-doped (La{sub 1-x}Ag{sub x}Mn{sub 0.9}Co{sub 0.1}O{sub 3}) and A-site deficient (La{sub 1-x}Mn{sub 0.9}Co{sub 0.1}O{sub 3-δ}) perovskites with x equal to 10, 20 and 30 at.% has been investigated in catalysts for soot combustion. The catalysts were prepared by the amorphous citrate method and characterized by XRD, nitrogen adsorption, XPS, O{sub 2}-TPD and TPR. The formationmore » of a rhombohedral excess-oxygen perovskite for Ag-doped and a cubic perovskite structure for an A-site deficient series is confirmed. The efficient catalytic performance of the larger Ag-doped perovskite structure is attributed to the rhombohedral crystalline structure, Ag{sub 2}O segregated phases and the redox pair Mn{sup 4+}/Mn{sup 3+}. A poor catalytic activity for soot combustion was observed with A-site deficient perovskites, despite the increase in the redox pair Mn{sup 4+}/Mn{sup 3+}, which is attributed to the cubic crystalline structure.« less

Fabrication of Water Jet Resistant and Thermally Stable Superhydrophobic Surfaces by Spray Coating of Candle Soot Dispersion.

PubMed

Qahtan, Talal F; Gondal, Mohammed A; Alade, Ibrahim O; Dastageer, Mohammed A

2017-08-08

A facile synthesis method for highly stable carbon nanoparticle (CNP) dispersion in acetone by incomplete combustion of paraffin candle flame is presented. The synthesized CNP dispersion is the mixture of graphitic and amorphous carbon nanoparticles of the size range of 20-50 nm and manifested the mesoporosity with an average pore size of 7 nm and a BET surface area of 366 m 2 g -1 . As an application of this material, the carbon nanoparticle dispersion was spray coated (spray-based coating) on a glass surface to fabricate superhydrophobic (water contact angle > 150° and sliding angle < 10 °) surfaces. The spray coated surfaces were found to exhibit much improved water jet resistance and thermal stability up to 400 °C compared to the surfaces fabricated from direct candle flame soot deposition (candle-based coating). This study proved that water jet resistant and thermally stable superhydrophobic surfaces can be easily fabricated by simple spray coating of CNP dispersion gathered from incomplete combustion of paraffin candle flame and this technique can be used for different applications with the potential for the large scale fabrication.

Potential contributions of asphalt and coal tar to black carbon quantification in urban dust, soils, and sediments

USGS Publications Warehouse

Yang, Y.; Mahler, B.J.; Van Metre, P.C.; Ligouis, B.; Werth, C.J.

2010-01-01

Measurements of black carbon (BC) using either chemical or thermal oxidation methods are generally thought to indicate the amount of char and/or soot present in a sample. In urban environments, however, asphalt and coal-tar particles worn from pavement are ubiquitous and, because of their pyrogenic origin, could contribute to measurements of BC. Here we explored the effect of the presence of asphalt and coal-tar particles on the quantification of BC in a range of urban environmental sample types, and evaluated biases in the different methods used for quantifying BC. Samples evaluated were pavement dust, residential and commercial area soils, lake sediments from a small urban watershed, and reference materials of asphalt and coal tar. Total BC was quantified using chemical treatment through acid dichromate (Cr2O7) oxidation and chemo-thermal oxidation at 375??C (CTO-375). BC species, including soot and char/charcoal, asphalt, and coal tar, were quantified with organic petrographic analysis. Comparison of results by the two oxidation methods and organic petrography indicates that both coal tar and asphalt contribute to BC quantified by Cr2O7 oxidation, and that coal tar contributes to BC quantified by CTO-375. These results are supported by treatment of asphalt and coal-tar reference samples with Cr2O7 oxidation and CTO-375. The reference asphalt is resistant to Cr2O7 oxidation but not to CTO-375, and the reference coal tar is resistant to both Cr2O7 oxidation and CTO-375. These results indicate that coal tar and/or asphalt can contribute to BC measurements in samples from urban areas using Cr2O7 oxidation or CTO-375, and caution is advised when interpreting BC measurements made with these methods. ?? 2010 Elsevier Ltd.

Effects of mixing states on the multiple-scattering properties of soot aerosols.

PubMed

Cheng, Tianhai; Wu, Yu; Gu, Xingfa; Chen, Hao

2015-04-20

The radiative properties of soot aerosols are highly sensitive to the mixing states of black carbon particles and other aerosol components. Light absorption properties are enhanced by the mixing state of soot aerosols. Quantification of the effects of mixing states on the scattering properties of soot aerosol are still not completely resolved, especially for multiple-scattering properties. This study focuses on the effects of the mixing state on the multiple scattering of soot aerosols using the vector radiative transfer model. Two types of soot aerosols with different mixing states such as external mixture soot aerosols and internal mixture soot aerosols are studied. Upward radiance/polarization and hemispheric flux are studied with variable soot aerosol loadings for clear and haze scenarios. Our study showed dramatic changes in upward radiance/polarization due to the effects of the mixing state on the multiple scattering of soot aerosols. The relative difference in upward radiance due to the different mixing states can reach 16%, whereas the relative difference of upward polarization can reach 200%. The effects of the mixing state on the multiple-scattering properties of soot aerosols increase with increasing soot aerosol loading. The effects of the soot aerosol mixing state on upwelling hemispheric flux are much smaller than in upward radiance/polarization, which increase with increasing solar zenith angle. The relative difference in upwelling hemispheric flux due to the different soot aerosol mixing states can reach 18% when the solar zenith angle is 75°. The findings should improve our understanding of the effects of mixing states on the optical properties of soot aerosols and their effects on climate. The mixing mechanism of soot aerosols is of critical importance in evaluating the climate effects of soot aerosols, which should be explicitly included in radiative forcing models and aerosol remote sensing.

Ozone adsorption on carbon nanoparticles

NASA Astrophysics Data System (ADS)

Chassard, Guillaume; Gosselin, Sylvie; Visez, Nicolas; Petitprez, Denis

2014-05-01

Carbonaceous particles produced by incomplete combustion or thermal decomposition of hydrocarbons are ubiquitous in the atmosphere. On these particles are adsorbed hundreds of chemical species. Those of great concern to health are polycyclic aromatic hydrocarbons (PAHs). During atmospheric transport, particulate PAHs react with gaseous oxidants. The induced chemical transformations may change toxicity and hygroscopicity of these potentially inhalable particles. The interaction between ozone and carbon particles has been extensively investigated in literature. However ozone adsorption and surface reaction mechanisms are still ambiguous. Some studies described a fast catalytic decomposition of ozone initiated by an atomic oxygen chemisorption followed by a molecular oxygen release [1-3]. Others suggested a reversible ozone adsorption according to Langmuir-type behaviour [4,5]. The aim of this present study is a better understanding of ozone interaction with carbon surfaces. An aerosol of carbon nanoparticles was generated by flowing synthetic air in a glass tube containing pure carbon (primary particles < 50 nm), under magnetic stirring. The aerosol was then mixed with ozone in an aerosol flow tube. Ozone uptake experiments were performed with different particles concentrations with a fixed ozone concentration. The influence of several factors on kinetics was examined: initial ozone concentration, particle size (50 nm ≤ Dp ≤ 200 nm) and competitive adsorption (with probe molecule and water). The effect of initial ozone concentration was first studied. Accordingly to literature, it has been observed that the number of gas-phase ozone molecules lost per unit particle surface area tends towards a plateau for high ozone concentration suggesting a reversible ozone adsorption according to a Langmuir mechanism. We calculated the initial reaction probability between O3 and carbon particles.An initial uptake coefficient of 1.10-4 was obtained. Similar experiments were realized by selecting the particles size with a differential mobility analyser. We observed a strong size-dependent increase in reactivity with the decrease of particles size. This result is relevant for the health issues. Indeed the smallest particles are most likely to penetrate deep into the lungs. Competitive reactions between ozone and other species like H2O or atomic oxygen were also considered. Oxygen atoms were generated by photolysis of O3 (or O2) and were chosen because it is believed to form the same reactive oxygen intermediates than ozone. A weak water physisorption on soot was observed revealing hydrophobic properties of particles. Oxygen atoms were found to be strongly reactive. A Langmuir behavior was observed for oxygen atoms adsorption on carbon particles and we were able to determine an initial uptake coefficient of approximately 2.10-2. [1] Fenidel, W., et al., Interaction between carbon or iron aerosol particles and ozone. Atmospheric Environment, 1995. 29(9): p. 967-973. [2] Smith, D. and A. Chughtai, Reaction kinetics of ozone at low concentrations with n-hexane soot. Journal of geophysical research, 1996. 101(D14): p. 19607-19,620. [3] Kamm, S., et al., The heterogeneous reaction of ozone with soot aerosol. Atmospheric Environment, 1999. 33(28): p. 4651-4661. [4] Stephens, S., M.J. Rossi, and D.M. Golden, The heterogeneous reaction of ozone on carbonaceous surfaces. International journal of chemical kinetics, 1986. 18(10): p. 1133-1149. [5] Pöschl, U., et al., Interaction of ozone and water vapor with spark discharge soot aerosol particles coated with benzo [a] pyrene: O3 and H2O adsorption, benzo [a] pyrene degradation, and atmospheric implications. The Journal of Physical Chemistry A, 2001. 105(16): p. 4029-4041.

Understanding the Role of a nano Ce Additive in the Size Distribution and Organic Composition of the Particulate Phase of Diesel Emissions

EPA Science Inventory

A number of alkali, alkaline earth, transition, and metalloid elements are known to act as fuel catalysts to limit the formation of soot precursors or promote its oxidation. These have been used with varying success on a variety of stationary and mobile combustion sources. Iron...

Aerothermal modeling program, phase 1

NASA Technical Reports Server (NTRS)

Srinivasan, R.; Reynolds, R.; Ball, I.; Berry, R.; Johnson, K.; Mongia, H.

1983-01-01

Aerothermal submodels used in analytical combustor models are analyzed. The models described include turbulence and scalar transport, gaseous full combustion, spray evaporation/combustion, soot formation and oxidation, and radiation. The computational scheme is discussed in relation to boundary conditions and convergence criteria. Also presented is the data base for benchmark quality test cases and an analysis of simple flows.

DFT studies on the heterogeneous oxidation of SO2 by oxygen functional groups on graphene.

PubMed

He, Guangzhi; He, Hong

2016-11-23

The heterogeneous oxidation of SO 2 has been the subject of intense scrutiny in atmospheric chemistry because of the adverse effects of sulfate particles. Although it has been found that the soot particles with a graphene-like structure play an important role in the oxidation of SO 2 , little is known about the atomic-level mechanism involved. Here, we studied the oxidation of SO 2 on oxygen-functionalized graphene using density functional theory (DFT) calculation. The results showed that SO 2 is oxidized by the epoxide group via a two-step mechanism, where the C-O bond away from the SO 2 is broken first, followed by the breaking of the other C-O bond and the synchronous formation of a new S-O bond. The energy barriers are significantly decreased when solvation free energies are involved, suggesting that humidity is favorable for promoting the oxidation by reducing the reaction barrier. The energy barriers for H 2 SO 3 oxidation are much higher than that for SO 2 oxidation, indicating that the direct conversion of SO 2 to SO 3 is the main pathway for the oxidation of SO 2 by oxygen-functionalized graphene sheets in both the gas phase and solution. The reduced density gradient (RDG) analysis showed that the hydrogen bond formed between H 2 SO 3 and epoxide groups enhances the stability of the reaction complex, and is responsible for the high energy barrier that has to be overcome for the reaction to proceed. These atomistic studies proposed a two-step mechanism for the oxidation of SO 2 on the oxygen-functionalized graphene-like carbonaceous surfaces under ambient conditions.

Ice nucleation activity of diesel soot particles at Cirrus relevant conditions: Effects of hydration, secondary organics coating, hydration, soot morphology, and coagulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kulkarni, Gourihar R.; China, Swarup; Liu, Shang

The role of atmospheric relevant soot particles that are processed in the atmosphere toward ice nucleation at cirrus cloud condition is poorly understood. In this study, the ice nucleating properties of diesel soot particles subjected to various physical and chemical aging treatments were investigated at temperatures ranging from -40 to -50 °C. We show that bare soot particles nucleate ice in deposition mode, but coating with secondary organics suppresses the heterogeneous ice nucleation potential of soot particles requiring homogeneous freezing threshold conditions. However, the ice nucleation efficiency of soot particles coated with an aqueous organic layer was similar to baremore » soot particles. Hydration of bare soot particles slightly enhanced the ice nucleation efficiency, and the IN abilities of compact soot particles (roundness = ~ 0.6) were similar to bare lacey soot particles (roundness = ~ 0.4). These results indicate that ice nucleation properties are sensitive to the various aging treatments.« less

Flexible conformable hydrophobized surfaces for turbulent flow drag reduction

NASA Astrophysics Data System (ADS)

Brennan, Joseph C.; Geraldi, Nicasio R.; Morris, Robert H.; Fairhurst, David J.; McHale, Glen; Newton, Michael I.

2015-05-01

In recent years extensive work has been focused onto using superhydrophobic surfaces for drag reduction applications. Superhydrophobic surfaces retain a gas layer, called a plastron, when submerged underwater in the Cassie-Baxter state with water in contact with the tops of surface roughness features. In this state the plastron allows slip to occur across the surface which results in a drag reduction. In this work we report flexible and relatively large area superhydrophobic surfaces produced using two different methods: Large roughness features were created by electrodeposition on copper meshes; Small roughness features were created by embedding carbon nanoparticles (soot) into Polydimethylsiloxane (PDMS). Both samples were made into cylinders with a diameter under 12 mm. To characterize the samples, scanning electron microscope (SEM) images and confocal microscope images were taken. The confocal microscope images were taken with each sample submerged in water to show the extent of the plastron. The hydrophobized electrodeposited copper mesh cylinders showed drag reductions of up to 32% when comparing the superhydrophobic state with a wetted out state. The soot covered cylinders achieved a 30% drag reduction when comparing the superhydrophobic state to a plain cylinder. These results were obtained for turbulent flows with Reynolds numbers 10,000 to 32,500.

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

NASA Astrophysics Data System (ADS)

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.

Development and Characterization of Laser-Induced Incandescence Towards Nanoparticle (Soot) Detection

NASA Technical Reports Server (NTRS)

VanderWal, Randy L.

2000-01-01

The production of particulates, notably soot, during combustion has both positive and negative ramifications. Exhaust from diesel engines under load (for example, shifting gears), flickering candle flames and fireplaces all produce soot leaving a flame. From an efficiency standpoint, emission of soot from engines, furnaces or even a simple flickering candle flame represents a loss of useful energy. The emission of soot from diesel engines, furnaces, power generation facilities, incinerators and even simple flames poses a serious environmental problem and health risk. Yet some industries intentionally produce soot as carbon black for use in inks, copier toner, tires and as pigments. Similarly, the presence of soot within flames can act both positively and negatively. Energy transfer from a combustion process is greatly facilitated by the radiative heat transfer from soot yet radiative heat transfer also facilitates the spread of unwanted fires. To understand soot formation and develop control strategies for soot emission/formation, measurements of soot concentration in both practical devices such as engines and controlled laboratory flames are necessary. Laser-induced incandescence (LII) has been developed and characterized to address this need, as described here.

Effects of PV Module Soiling on Glass Surface Resistance and Potential-Induced Degradation: Preprint

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hacke, Peter; Burton, Patrick; Hendrickson, Alex

2015-12-03

The sheet resistance of three soil types (Arizona road dust, soot, and sea salt) on glass were measured by the transmission line method as a function of relative humidity (RH) between 39% and 95% at 60 degrees C. Sea salt yielded a 3.5 order of magnitude decrease in resistance on the glass surface when the RH was increased over this RH range. Arizona road dust showed reduced sheet resistance at lower RH, but with less humidity sensitivity over the range tested. The soot sample did not show significant resistivity change compared to the unsoiled control. Photovoltaic modules with sea saltmore » on their faces were step-stressed between 25% and 95% RH at 60 degrees C applying -1000 V bias to the active cell circuit. Leakage current from the cell circuit to ground ranged between two and ten times higher than that of the unsoiled controls. Degradation rate of modules with salt on the surface increased with increasing RH and time.« less

Global climate change driven by soot at the K-Pg boundary as the cause of the mass extinction

NASA Astrophysics Data System (ADS)

Kaiho, Kunio; Oshima, Naga; Adachi, Kouji; Adachi, Yukimasa; Mizukami, Takuya; Fujibayashi, Megumu; Saito, Ryosuke

2016-07-01

The mass extinction of life 66 million years ago at the Cretaceous/Paleogene boundary, marked by the extinctions of dinosaurs and shallow marine organisms, is important because it led to the macroevolution of mammals and appearance of humans. The current hypothesis for the extinction is that an asteroid impact in present-day Mexico formed condensed aerosols in the stratosphere, which caused the cessation of photosynthesis and global near-freezing conditions. Here, we show that the stratospheric aerosols did not induce darkness that resulted in milder cooling than previously thought. We propose a new hypothesis that latitude-dependent climate changes caused by massive stratospheric soot explain the known mortality and survival on land and in oceans at the Cretaceous/Paleogene boundary. The stratospheric soot was ejected from the oil-rich area by the asteroid impact and was spread globally. The soot aerosols caused sufficiently colder climates at mid-high latitudes and drought with milder cooling at low latitudes on land, in addition to causing limited cessation of photosynthesis in global oceans within a few months to two years after the impact, followed by surface-water cooling in global oceans in a few years. The rapid climate change induced terrestrial extinctions followed by marine extinctions over several years.

Global climate change driven by soot at the K-Pg boundary as the cause of the mass extinction

PubMed Central

Kaiho, Kunio; Oshima, Naga; Adachi, Kouji; Adachi, Yukimasa; Mizukami, Takuya; Fujibayashi, Megumu; Saito, Ryosuke

2016-01-01

The mass extinction of life 66 million years ago at the Cretaceous/Paleogene boundary, marked by the extinctions of dinosaurs and shallow marine organisms, is important because it led to the macroevolution of mammals and appearance of humans. The current hypothesis for the extinction is that an asteroid impact in present-day Mexico formed condensed aerosols in the stratosphere, which caused the cessation of photosynthesis and global near-freezing conditions. Here, we show that the stratospheric aerosols did not induce darkness that resulted in milder cooling than previously thought. We propose a new hypothesis that latitude-dependent climate changes caused by massive stratospheric soot explain the known mortality and survival on land and in oceans at the Cretaceous/Paleogene boundary. The stratospheric soot was ejected from the oil-rich area by the asteroid impact and was spread globally. The soot aerosols caused sufficiently colder climates at mid–high latitudes and drought with milder cooling at low latitudes on land, in addition to causing limited cessation of photosynthesis in global oceans within a few months to two years after the impact, followed by surface-water cooling in global oceans in a few years. The rapid climate change induced terrestrial extinctions followed by marine extinctions over several years. PMID:27414998

Global climate change driven by soot at the K-Pg boundary as the cause of the mass extinction.

PubMed

Kaiho, Kunio; Oshima, Naga; Adachi, Kouji; Adachi, Yukimasa; Mizukami, Takuya; Fujibayashi, Megumu; Saito, Ryosuke

2016-07-14

The mass extinction of life 66 million years ago at the Cretaceous/Paleogene boundary, marked by the extinctions of dinosaurs and shallow marine organisms, is important because it led to the macroevolution of mammals and appearance of humans. The current hypothesis for the extinction is that an asteroid impact in present-day Mexico formed condensed aerosols in the stratosphere, which caused the cessation of photosynthesis and global near-freezing conditions. Here, we show that the stratospheric aerosols did not induce darkness that resulted in milder cooling than previously thought. We propose a new hypothesis that latitude-dependent climate changes caused by massive stratospheric soot explain the known mortality and survival on land and in oceans at the Cretaceous/Paleogene boundary. The stratospheric soot was ejected from the oil-rich area by the asteroid impact and was spread globally. The soot aerosols caused sufficiently colder climates at mid-high latitudes and drought with milder cooling at low latitudes on land, in addition to causing limited cessation of photosynthesis in global oceans within a few months to two years after the impact, followed by surface-water cooling in global oceans in a few years. The rapid climate change induced terrestrial extinctions followed by marine extinctions over several years.

A morphological investigation of soot produced by the detonation of munitions.

PubMed

Pantea, Dana; Brochu, Sylvie; Thiboutot, Sonia; Ampleman, Guy; Scholz, Günter

2006-10-01

The morphology of three different detonation soot samples along with other common soot materials such as carbon black, diesel soot and chimney soot was studied by elemental and proximate analysis, X-ray diffraction and electron microscopy. The goal of this study was to better define the morphology of the detonation soot in order to better assess the interactions of this type of soot with explosive residues. The detonation soot samples were obtained by the detonation of artillery 155mm projectiles filled with either pure TNT (2,4,6-trinitrotoluene) or composition B, a military explosive based on a mixture of TNT and RDX (trimethylentrinitramine). The carbon content of the soot samples varied considerably depending on the feedstock composition. Detonation soot contains less carbon and more nitrogen than the other carbonaceous samples studied, due to the molecular structure of the energetic materials detonated such as TNT and RDX. The ash concentration was higher for detonation soot samples due to the high metal content coming from the projectiles shell and to the soil contamination which occurred during the detonation. By X-ray diffraction, diamond and graphite were found to be the major crystalline carbon forms in the detonation soot. Two electron microscopy techniques were used in this study to visualise the primary particles and to try to explain the formation mechanism of detonation soot samples.

Sooting turbulent jet flame: characterization and quantitative soot measurements

NASA Astrophysics Data System (ADS)

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.

Structure and Composition of Air-Plane Soots and Surrogates Analyzed by Raman Spectroscopy and Laser/Ions Desorption Mass Spectrometry

NASA Astrophysics Data System (ADS)

Ortega, Ismael; Chazallon, Bertrand; Carpentier, Yvain; Irimiea, Cornelia; Focsa, Cristian; Ouf, François-Xavier; Salm, François; Delhaye, David; Gaffié, Daniel; Yon, Jérôme

2015-04-01

Aviation alters the composition of the atmosphere globally and can thus drive climate change and ozone depletion [1]. An aircraft exhaust plume contains species emitted by the engines, species formed in the plume from the emitted species and atmospheric species that become entrained into the plume. The majority of emitted species (gases and soot particles) are produced by the combustion of kerosene with ambient air in the combustion chamber of the engine. Emissions of soot particles by air-planes produce persistent contrails in the upper troposphere in ice-supersaturated air masses that contribute to cloudiness and impact the radiative properties of the atmosphere. These aerosol-cloud interactions represent one of the largest sources of uncertainty in global climate models [2]. Though the formation of atmospheric ice particles has been studied since many years [3], there are still numerous opened questions on nucleation properties of soot particles [4], as the ice nucleation experiments showed a large spread in results depending on the nucleation mode chosen and origin of the soot produced. Most likely one of the reasons behind these discrepancies resides in the different physico-chemical properties (composition, structure) of soot particles produced in different conditions, e.g. with respect to fuel or combustion techniques. In this work, we use Raman microscopy (266, 514 and 785 nm excitation) and ablation techniques (SIMS, Secondary Ions Mass Spectrometry, and Laser Desorption Mass Spectrometry) to characterize soot particles produced from air-plane at different engine regimes simulating a landing and taking-off (LTO) cycle. First, the spectral parameters of the first-order Raman band of various soot samples, collected from three different sources in the frame of the MERMOSE project (http://mermose.onera.fr/): PowerJet SaM-146 turbofan (four engine regimes), CAST generator (propane fuel, four different global equivalence ratios), and Kerosene laboratory flame are provided. The spectra are analyzed by performing a de-convolution using the approach described by Sadezky et al. (2005). The soot obtained at different engine regimes presents very similar spectra, with the only exception of the soot obtained at 30% engine regime. In this case, the contribution of D2 band is similar to the contribution of D3 band, while for the samples obtained at 70%, 85% and 100% engine regimes D3 contribution is larger. The results point to a very little impact of engine regime on the generated soot structure. In contrast, surrogate soots show a dependence on the initial combustion parameters and collection conditions. Second, the surface chemical composition of the soot particles with special focus on PAHs are analyzed by two-Step (Desorption/Ionization) Laser Mass Spectrometry (L2MS) and Time of Fight Secondary Ion Mass Spectrometry (ToF-SIMS) techniques. In L2MS, the adsorbed phase is probed by nanosecond laser desorption (λd=532nm), then the ejected molecules are ionized with a second ns laser (λi=266nm) and further mass-separated by ToF-MS. In both techniques the spectra are obtained using positive polarity, which is better suited for detection of PAHs. A good agreement was obtained between the two techniques for the total PAH content of the analyzed samples. Moreover, the total PAH content followed the same trend as the OC/EC ratio measured with a thermo-optic analyzer (Improve protocol): the 30% engine regime soot presents a high concentration of PAHs and a high OC content, while the three other regimes give a relatively low content of PAHs and OC. References [1] Lee et al., Atmos. Env. 44, 4678-4734, 2010 [2] IPCC 2014, Chap7: http://www.ipcc.ch [3] L. Dufour, Ciel et Terre, vol 82, p1-36, 1966 [4] C. Hoose & O. Möhler, Atmos.Chem.Phys. 12, 9817-9854, 2012 [5] Sadezky, et al., Carbon, 43, 1731-1742, 2005

Nitrous acid in a street canyon environment: sources and the contribution to local oxidation capacity

NASA Astrophysics Data System (ADS)

Yun, Hui; Wang, Zhe; Zha, Qiaozhi; Wang, Weihao; Xue, Likun; Zhang, Li; Li, Qinyi; Cui, Long; Lee, Shuncheng; Poon, Steven; Wang, Tao

2017-04-01

Nitrous acid (HONO) is one of the dominant sources of hydroxyl radical (OH) and plays an important role in photochemical oxidation processes in the atmosphere. Even though HONO has been extensively studied in urban areas, its importance and effects in street canyon microenvironment has not been thoroughly investigated. Street canyons which suffer serious air pollution problem are widely distributed in downtown areas with paralleled high buildings and narrow roads in the center. In this study, we measured HONO at a roadside of a street canyon in urban Hong Kong and applied an observation-based box model based on Master Chemical Mechanism (MCM 3.3) to investigate the contribution of HONO to local oxidation chemistry. Higher HONO mixing ratios were observed in the daytime than in the nighttime. An average emission ratio (ΔHONO/ΔNOx) of 1.0% (±0.5%) was derived at this roadside site and the direct HONO emission from vehicles contributed to 38% of the measured HONO in the street canyon. Heterogeneous NO2 conversion on humid ground or building surfaces and the uptake of NO2 on fresh soot surfaces were the other two important HONO sources in this microenvironment. OBM simulations constrained with observed HONO showed that the peak concentration of OH, HO2 and RO2 is 7.9, 5.0 and 7.5 times of the result in the case with only OH+NO as HONO source. Photolysis of HONO contributed to 86.5% of the total primary radical production rates and can lead to efficient NO2 and O3 production under the condition of weak regional O3 transport. Our study suggests that HONO could significantly increase the atmospheric oxidation capacity in a street canyon which may impact the secondary formation of aerosols and OVOCs.

Electrically heated particulate matter filter soot control system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gonze, Eugene V.; Paratore, Jr., Michael J.; Bhatia, Garima

A regeneration system includes a particulate matter (PM) filter with an upstream end for receiving exhaust gas and a downstream end. A control module determines a current soot loading level of the PM filter and compares the current soot loading level to a predetermined soot loading level. The control module permits regeneration of the PM filter when the current soot loading level is less than the predetermined soot loading level.

Investigation of in-flame soot optical properties in laminar coflow diffusion flames using thermophoretic particle sampling and spectral light extinction

NASA Astrophysics Data System (ADS)

Kempema, Nathan J.; Ma, Bin; Long, Marshall B.

2016-09-01

Soot optical properties are essential to the noninvasive study of the in-flame evolution of soot particles since they allow quantitative interpretation of optical diagnostics. Such experimental data are critical for comparison to results from computational models and soot sub-models. In this study, the thermophoretic sampling particle diagnostic (TSPD) technique is applied along with data from a previous spectrally resolved line-of-sight light attenuation experiment to determine the soot volume fraction and absorption function. The TSPD technique is applied in a flame stabilized on the Yale burner, and the soot scattering-to-absorption ratio is calculated using the Rayleigh-Debye-Gans theory for fractal aggregates and morphology information from a previous sampling experiment. The soot absorption function is determined as a function of wavelength and found to be in excellent agreement with previous in-flame measurements of the soot absorption function in coflow laminar diffusion flames. Two-dimensional maps of the soot dispersion exponent are calculated and show that the soot absorption function may have a positive or negative exponential wavelength dependence depending on the in-flame location. Finally, the wavelength dependence of the soot absorption function is related to the ratio of soot absorption functions, as would be found using two-excitation-wavelength laser-induced incandescence.

Ice nucleation activity of diesel soot particles at cirrus relevant temperature conditions: Effects of hydration, secondary organics coating, soot morphology, and coagulation

NASA Astrophysics Data System (ADS)

Kulkarni, Gourihar; China, Swarup; Liu, Shang; Nandasiri, Manjula; Sharma, Noopur; Wilson, Jacqueline; Aiken, Allison C.; Chand, Duli; Laskin, Alexander; Mazzoleni, Claudio; Pekour, Mikhail; Shilling, John; Shutthanandan, Vaithiyalingam; Zelenyuk, Alla; Zaveri, Rahul A.

2016-04-01

Ice formation by diesel soot particles was investigated at temperatures ranging from -40 to -50°C. Size-selected soot particles were physically and chemically aged in an environmental chamber, and their ice nucleating properties were determined using a continuous flow diffusion type ice nucleation chamber. Bare (freshly formed), hydrated, and compacted soot particles, as well as α-pinene secondary organic aerosol (SOA)-coated soot particles at high relative humidity conditions, showed ice formation activity at subsaturation conditions with respect to water but below the homogeneous freezing threshold conditions. However, SOA-coated soot particles at dry conditions were observed to freeze at homogeneous freezing threshold conditions. Overall, our results suggest that heterogeneous ice nucleation activity of freshly emitted diesel soot particles are sensitive to some of the aging processes that soot can undergo in the atmosphere.

Corrosive Space Gas Restores Artwork, Promises Myriad Applications

NASA Technical Reports Server (NTRS)

2007-01-01

Atomic oxygen's unique characteristic of oxidizing primarily hydrogen, carbon, and hydrocarbon polymers at surface levels has been applied in the restoration of artwork, detection of document forgeries, and removal of bacterial contaminants from surgical implants. The Electro-Physics Branch at Glenn Research Center built on corrosion studies of long-duration coatings for use in space, and applied atomic oxygen's selectivity to instances where elements need to be removed from a surface. Atomic oxygen is able to remove organic compounds high in carbon (mostly soot) from fire-damaged artworks without causing a shift in the paint color. First successfully tested on oil paintings, the team then applied the restoration technique to acrylics, watercolors, and ink. The successful art restoration process was well-publicized, and soon a multinational, nonprofit professional organization dedicated to the art of forensic analysis of documents had successfully applied this process in the field of forgery detection. The gas has biomedical applications as well-Atomic Oxygen technology can be used to decontaminate orthopedic surgical hip and knee implants prior to surgery, and additional collaborative research between the Cleveland Clinic Foundation and the Glenn team shows that this gas's roughening of surfaces improves cell adhesion, which is important for the development of new drugs.

Measuring and predicting sooting tendencies of oxygenates, alkanes, alkenes, cycloalkanes, and aromatics on a unified scale

DOE PAGES

Das, Dhrubajyoti D.; St. John, Peter C.; McEnally, Charles S.; ...

2017-12-27

Databases of sooting indices, based on measuring some aspect of sooting behavior in a standardized combustion environment, are useful in providing information on the comparative sooting tendencies of different fuels or pure compounds. However, newer biofuels have varied chemical structures including both aromatic and oxygenated functional groups, which expands the chemical space of relevant compounds. In this work, we propose a unified sooting tendency database for pure compounds, including both regular and oxygenated hydrocarbons, which is based on combining two disparate databases of yield-based sooting tendency measurements in the literature. Unification of the different databases was made possible by leveragingmore » the greater dynamic range of the color ratio pyrometry soot diagnostic. This unified database contains a substantial number of pure compounds (≥ 400 total) from multiple categories of hydrocarbons important in modern fuels and establishes the sooting tendencies of aromatic and oxygenated hydrocarbons on the same numeric scale for the first time. Then, using this unified sooting tendency database, we have developed a predictive model for sooting behavior applicable to a broad range of hydrocarbons and oxygenated hydrocarbons. The model decomposes each compound into single-carbon fragments and assigns a sooting tendency contribution to each fragment based on regression against the unified database. The model’s predictive accuracy (as demonstrated by leave-one-out cross-validation) is comparable to a previously developed, more detailed predictive model. The fitted model provides insight into the effects of chemical structure on soot formation, and cases where its predictions fail reveal the presence of more complicated kinetic sooting mechanisms. Our work will therefore enable the rational design of low-sooting fuel blends from a wide range of feedstocks and chemical functionalities.« less

Measuring and predicting sooting tendencies of oxygenates, alkanes, alkenes, cycloalkanes, and aromatics on a unified scale

DOE Office of Scientific and Technical Information (OSTI.GOV)

Das, Dhrubajyoti D.; St. John, Peter C.; McEnally, Charles S.

Databases of sooting indices, based on measuring some aspect of sooting behavior in a standardized combustion environment, are useful in providing information on the comparative sooting tendencies of different fuels or pure compounds. However, newer biofuels have varied chemical structures including both aromatic and oxygenated functional groups, which expands the chemical space of relevant compounds. In this work, we propose a unified sooting tendency database for pure compounds, including both regular and oxygenated hydrocarbons, which is based on combining two disparate databases of yield-based sooting tendency measurements in the literature. Unification of the different databases was made possible by leveragingmore » the greater dynamic range of the color ratio pyrometry soot diagnostic. This unified database contains a substantial number of pure compounds (≥ 400 total) from multiple categories of hydrocarbons important in modern fuels and establishes the sooting tendencies of aromatic and oxygenated hydrocarbons on the same numeric scale for the first time. Then, using this unified sooting tendency database, we have developed a predictive model for sooting behavior applicable to a broad range of hydrocarbons and oxygenated hydrocarbons. The model decomposes each compound into single-carbon fragments and assigns a sooting tendency contribution to each fragment based on regression against the unified database. The model’s predictive accuracy (as demonstrated by leave-one-out cross-validation) is comparable to a previously developed, more detailed predictive model. The fitted model provides insight into the effects of chemical structure on soot formation, and cases where its predictions fail reveal the presence of more complicated kinetic sooting mechanisms. Our work will therefore enable the rational design of low-sooting fuel blends from a wide range of feedstocks and chemical functionalities.« less

Soot formation and burnout in flames

NASA Technical Reports Server (NTRS)

Prado, B.; Bittner, J. D.; Neoh, K.; Howard, J. B.

1980-01-01

The amount of soot formed when burning a benzene/hexane mixture in a turbulent combustor was examined. Soot concentration profiles in the same combustor for kerosene fuel are given. The chemistry of the formation of soot precursors, the nucleation, growth and subsequent burnout of soot particles, and the effect of mixing on the previous steps were considered.

Computational modeling of soot nucleation

NASA Astrophysics Data System (ADS)

Chung, Seung-Hyun

Recent studies indicate that soot is the second most significant driver of climate change---behind CO2, but ahead of methane---and increased levels of soot particles in the air are linked to health hazards such as heart disease and lung cancer. Within the soot formation process, soot nucleation is the least understood step, and current experimental findings are still limited. This thesis presents computational modeling studies of the major pathways of the soot nucleation process. In this study, two regimes of soot nucleation---chemical growth and physical agglomeration---were evaluated and the results demonstrated that combustion conditions determine the relative importance of these two routes. Also, the dimerization process of polycyclic aromatic hydrocarbons, which has been regarded as one of the most important physical agglomeration processes in soot formation, was carefully examined with a new method for obtaining the nucleation rate using molecular dynamics simulation. The results indicate that the role of pyrene dimerization, which is the commonly accepted model, is expected to be highly dependent on various flame temperature conditions and may not be a key step in the soot nucleation process. An additional pathway, coronene dimerization in this case, needed to be included to improve the match with experimental data. The results of this thesis provide insight on the soot nucleation process and can be utilized to improve current soot formation models.

The single scattering properties of soot aggregates with concentric core-shell spherical monomers

NASA Astrophysics Data System (ADS)

Wu, Yu; Cheng, Tianhai; Gu, Xingfa; Zheng, Lijuan; Chen, Hao; Xu, Hui

2014-03-01

Anthropogenic soot aerosols are shown as complex, fractal-like aggregated structures with high light absorption efficiency. In atmospheric environment, soot monomers may tend to acquire a weakly absorbing coating, such as an organic coating, which introduces further complexity to the optical properties of the aggregates. The single scattering properties of soot aggregates can be significantly influenced by the coated status of these kinds of aerosols. In this article, the monomers of fractal soot aggregates are modelled as semi-external mixtures (physical contact) with constant radius of soot core and variable sizes of the coating for specific soot volume fractions. The single scattering properties of these coated soot particles, such as phase function, the cross sections of extinction and absorption, single scattering albedo (SSA) and asymmetry parameter (ASY), are calculated using the numerically exact superposition T-matrix method. The random-orientation averaging results have shown that the single scattering properties of these coated soot aggregates are significantly different from the single volume-equivalent core-shell sphere approximation using the Mie theory and the homogeneous aggregates with uncoated monomers using the effective medium theory, such as Maxwell-Garnett and Bruggemann approximations, which overestimate backscattering of coated soot. It is found that the SSA and cross sections of extinction and absorption are increased for soot aggregates with thicker weakly absorbing coating on the monomers. Especially, the SSA values of these simulated aggregates with less soot core volume fractions are remarkably (~50% for core volume fraction of soot aggregates of 0.5, ~100% for a core volume fraction of 0.2, at 0.67 μm) larger than for uncoated soot particles without consideration of coating. Moreover, the cross sections of extinction and absorption are underestimated by the computation of equivalent homogeneous fractal aggregate approximation (within 5% for the T-matrix method and 10-25% for the Rayleigh-Debye-Gans approximation due to different soot volume fractions). Further understanding of the optical properties of these coated soot aggregates would be helpful for both environment monitoring and climate studies.

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

NASA Astrophysics Data System (ADS)

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 < -38 °C (cirrus could regime). Nevertheless, we question if this is caused by a heterogeneous phase change due the presence of a so called active site or due to pore-condensation of water as predicted by the inverse Kelvin effect followed by homogeneous 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.

Characteristics of individual particles in Beijing before, during and after the 2014 APEC meeting

NASA Astrophysics Data System (ADS)

Xu, Zhongjun; Shan, Wei; Qi, Tao; Gao, Jian

2018-05-01

To understand the characteristics of individual aerosol particles as well as the effects of emission control measures on the air quality in Beijing before, during and after the 2014 APEC meeting, aerosol samples collected in Beijing from Oct. 8 to Nov. 24 were investigated by a scanning electron microscopy (SEM) coupled with an energy-dispersive X-ray (EDX). Individual particles were classified into fly ash, ammonium sulfate, carbonaceous particle, tar ball, soot aggregates, Fe/Ti oxide, Ca/Mg carbonate, calcium sulfate and aluminosilicates/quartz. The results showed that PM0.5-1.0 was predominant in aerosol particles while PM2.5-10 was the fewest in aerosol particles. Soot aggregates and carbonaceous particles mainly located in the size range of 0.5-2.5 μm and mineral particles were dominant in the size range of 2.5-10 μm. The tough emission control measures taken by the local government greatly improved the air quality. Reducing vehicles on the roads substantially decreased the amount of soot aggregates, and restricting coal combustion decreased the amount of tar ball during the APEC meeting. The concentrations of carbonaceous and mineral particles abated probably owing to the control on VOCs emission, and water spray and demolition layoff, respectively, during the APEC meeting.

Potential Climate and Ozone Impacts From Hybrid Rocket Engine Emissions

NASA Astrophysics Data System (ADS)

Ross, M.

2009-12-01

Hybrid rocket engines that use N2O as an oxidizer and a solid hydrocarbon (such as rubber) as a fuel are relatively new. Little is known about the composition of such hybrid engine emissions. General principles and visual inspection of hybrid plumes suggest significant soot and possibly NO emissions. Understanding hybrid rocket emissions is important because of the possibility that a fleet of hybrid powered suborbital rockets will be flying on the order of 1000 flights per year by 2020. The annual stratospheric emission for these rockets would be about 10 kilotons, equal to present day solid rocket motor (SRM) emissions. We present a preliminary analysis of the magnitude of (1) the radiative forcing from soot emissions and (2) the ozone depletion from soot and NO emissions associated with such a fleet of suborbital hybrid rockets. Because the details of the composition of hybrid emissions are unknown, it is not clear if the ozone depletion caused by these hybrid rockets would be more or less than the ozone depletion from SRMs. We also consider the climate implications associated with the N2O production and use requirements for hybrid rockets. Finally, we identify the most important data collection and modeling needs that are required to reliably assess the complete range of environmental impacts of a fleet of hybrid rockets.

Turbulent Flame Processes Via Diffusion Flame-Vortex Ring Interactions

NASA Technical Reports Server (NTRS)

Dahm, Werner J. A.; Chen, Shin-Juh; Silver, Joel A.; Piltch, Nancy D.; VanderWal, Randall L.

2001-01-01

Flame-vortex interactions are canonical configurations that can be used to study the underlying processes occurring in turbulent reacting flows. This configuration contains many of the fundamental aspects of the coupling between fluid dynamics and combustion that could be investigated with more controllable conditions than are possible under direct investigations of turbulent flames. Diffusion flame-vortex ring interaction contains many of the fundamental elements of flow, transport, combustion, and soot processes found in turbulent diffusion flames. Some of these elements include concentrated vorticity, entrainment and mixing, strain and nonequilibrium phenomena, diffusion and differential diffusion, partial premixing and diluent effects, soot formation and oxidation, and heat release effects. Such simplified flowfield allows the complex processes to be examined more closely and yet preserving the physical processes present in turbulent reacting flows. Furthermore, experimental results from the study of flame-vortex interactions are useful for the validation of numerical simulations and more importantly to deepen our understanding of the fundamental processes present in reacting flows. Experimental and numerical results obtained under microgravity conditions of the diffusion flame-vortex ring interaction are summarized in this paper. Results are obtained using techniques that include Flame Luminosity Imaging (FLI), Laser Soot-Mie Scattering (LSMS), Computational Fluid Dynamics and Combustion (CFDC), and Diode Laser Spectroscopy/Iterative Temperature with Assumed Chemistry (DLS/ITAC).

Effect of Morphology and Composition on the Hygroscopicity of Soot Aerosols

NASA Astrophysics Data System (ADS)

Williams, L.; Slowik, J.; Davidovits, P.; Jayne, J.; Kolb, C.; Worsnop, D.; Rudich, Y.

2003-12-01

Freshly generated soot aerosols are initially hydrophobic and unlikely to act as cloud condensation nuclei (CCN). However, during combustion many low vapor pressure gas products are formed that may then condense on existing soot aerosols. Additionally, soot particles may acquire coatings as they age, such as acids, salts, and oxygenated organics. An understanding of this aging process and its effect on soot hygroscopicity is necessary to address the potential of soot to act as a CCN. The transformation of soot from hydrophobic to hydrophilic is the focus of this work. An aim here is to determine the minimum coating required for hygroscopic growth. Soot particles produced by combustion of mixtures of fuel and air are size selected by a Differential Mobility Analyzer (DMA) and entrained in a laminar flow passing through a flow tube. The size selected soot particles are mixed with a controlled amount of the gas phase precursors to produce the coatings to be studied. Initial studies are focused on coatings of H2SO4, NH4NO3, and selected organics. The number of particles per unit volume of air is counted by a Condensation Particle Counter (CPC) and the particles are isokinetically sampled into an Aerosol Mass Spectrometer (AMS). Two distinct types of soot aerosols have been observed depending on the type of fuel and air mixture. With soot produced by the combustion of propane and air, the AMS shows a polydisperse particle size distribution with aerodynamic diameters ranging from 100 nm to 400 nm. The aerodynamic diameter is linearly related to the DMA-determined mobility diameter with the product density x shape factor = 1.2. The organic molecules in this soot are mostly PAH compounds. However, when kerosene is added to the propane flame, the soot particle morphology and composition is strikingly altered. While the DMA shows an essentially unchanged mobility diameter distribution, in the range 100 nm to 400, aerodynamic particle diameter is constant at about 100 nm, independent of the mobility diameter. This type of constancy of the aerodynamic diameter has been observed for soot particles in diesel engine exhaust and has been interpreted in terms of a size-dependent effective density. The soot chemical composition is also altered. In this soot the organics are mainly linear hydrocarbons. The differences between these two types of soot with respect to hygroscopicity and effective area are being investigated.

Soot Formation in Hydrocarbon/Air Laminar Jet Diffusion Flames

NASA Technical Reports Server (NTRS)

Sunderland, P. B.; Faeth, G. M.

1994-01-01

Soot processes within hydrocarbon/air diffusion flames are important because they affect the durability and performance of propulsion systems, the hazards of unwanted fires, the pollutant and particulate emissions from combustion processes, and the potential for developing computational combustion. Motivated by these observations, this investigation involved an experimental study of the structure and soot properties of round laminar jet diffusion flames, seeking an improved understanding of soot formation (growth and nucleation) within diffusion flames. The present study extends earlier work in this laboratory concerning laminar smoke points (l) and soot formation in acetylene/air laminar jet diffusion flames (2), emphasizing soot formation in hydrocarbon/air laminar jet diffusion flames for fuels other than acetylene. In the flame system, acetylene is the dominant gas species in the soot formation region and both nucleation and growth were successfully attributed to first-order reactions of acetylene, with nucleation exhibiting an activation energy of 32 kcal/gmol while growth involved negligible activation energy and a collision efficiency of O.53%. In addition, soot growth in the acetylene diffusion flames was comparable to new soot in premixed flame (which also has been attributed to first-order acetylene reactions). In view of this status, a major issue is the nature of soot formation processes in diffusion flame involving hydrocarbon fuels other than acetylene. In particular, information is needed about th dominant gas species in the soot formation region and the impact of gas species other than acetylene on soot nucleation and growth.

An Experimental Investigation of the Laminar Flamelet Concept for Soot Properties

NASA Technical Reports Server (NTRS)

Diez, F. J.; Aalburg, C.; Sunderland, P. B.; Urban, D. L.; Yuan, Z.-G.; Faeth, G. M.

2007-01-01

The soot properties of round, nonbuoyant, laminar jet diffusion flames are described, based on experiments at microgravity carried out on orbit during three flights of the Space Shuttle Columbia, (Flights STS-83, 94 and 107). Experimental conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K and ambient pressures of 35-100 kPa. Measurements included soot volume fraction distributions using deconvoluted laser extinction imaging, and soot temperature distributions using deconvoluted multiline emission imaging. Flowfield modeling based on the work of Spalding is presented. The present work explores whether soot properties of these flames are universal functions of mixture fraction, i.e., whether they satisfy soot state relationships. Measurements are presented, including radiative emissions and distributions of soot temperature and soot volume fraction. It is shown that most of the volume of these flames is bounded by the dividing streamline and thus should follow residence time state relationships. Most streamlines from the fuel supply to the surroundings are found to exhibit nearly the same maximum soot volume fraction and temperature. The radiation intensity along internal streamlines also is found to have relatively uniform values. Finally, soot state relationships were observed, i.e., soot volume fraction was found to correlate with estimated mixture fraction for each fuel/pressure selection. These results support the existence of soot property state relationships for steady nonbuoyant laminar diffusion flames, and thus in a large class of practical turbulent diffusion flames through the application of the laminar flamelet concept.

Thermophysics Characterization of Kerosene Combustion

NASA Technical Reports Server (NTRS)

Wang, Ten-See

2000-01-01

A one-formula surrogate fuel formulation and its quasi-global combustion kinetics model are developed to support the design of injectors and thrust chambers of kerosene-fueled rocket engines. This surrogate fuel model depicts a fuel blend that properly represents the general physical and chemical properties of kerosene. The accompanying gaseous-phase thermodynamics of the surrogate fuel is anchored with the heat of formation of kerosene and verified by comparing a series of one-dimensional rocket thrust chamber calculations. The quasi-global combustion kinetics model consists of several global steps for parent fuel decomposition, soot formation, and soot oxidation, and a detailed wet-CO mechanism. The final thermophysics formulations are incorporated with a computational fluid dynamics model for prediction of the combustor efficiency of an uni-element, tri-propellant combustor and the radiation of a kerosene-fueled thruster plume. The model predictions agreed reasonably well with those of the tests.

Removal of ozone on clean, dusty and sooty supply air filters

NASA Astrophysics Data System (ADS)

Hyttinen, Marko; Pasanen, Pertti; Kalliokoski, Pentti

The removal of ozone (O 3) on supply air filters was studied. Especially, the effects of dust load, diesel soot, relative humidity (RH), and exposure time on the removal of O 3 were investigated. Some loss of O 3 was observed in all the filters, except in an unused G3 pre-filter made of polyester. Dust load and quality influenced the reduction of O 3; especially, diesel soot removed O 3 effectively. Increasing the RH resulted in a larger O 3 removal. The removal of O 3 was highest in the beginning of the test, but it declined within 2 h reaching almost a steady state as the exposure continued. However, the sooty filters continued to remove as much as 25-30% of O 3. Up to 11% of O 3 removed participated in the production of formaldehyde. Small amounts of other oxidation products were also detected.

Laminar Premixed and Diffusion Flames (Ground-Based Study)

NASA Technical Reports Server (NTRS)

Dai, Z.; El-Leathy, A. M.; Lin, K.-C.; Sunderland, P. B.; Xu, F.; Faeth, G. M.; Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2000-01-01

Ground-based studies of soot processes in laminar flames proceeded in two phases, considering laminar premixed flames and laminar diffusion flames, in turn. The test arrangement for laminar premixed flames involved round flat flame burners directed vertically upward at atmospheric pressure. The test arrangement for laminar jet diffusion flames involved a round fuel port directed vertically upward with various hydrocarbon fuels burning at atmospheric pressure in air. In both cases, coflow was used to prevent flame oscillations and measurements were limited to the flame axes. The measurements were sufficient to resolve soot nucleation, growth and oxidation rates, as well as the properties of the environment needed to evaluate mechanisms of these processes. The experimental methods used were also designed to maintain capabilities for experimental methods used in corresponding space-based experiments. This section of the report will be limited to consideration of flame structure for both premixed and diffusion flames.

Thermophysics Characterization of Kerosene Combustion

NASA Technical Reports Server (NTRS)

Wang, Ten-See

2001-01-01

A one-formula surrogate fuel formulation and its quasi-global combustion kinetics model are developed to support the design of injectors and thrust chambers of kerosene-fueled rocket engines. This surrogate fuel model depicts a fuel blend that properly represents the general physical and chemical properties of kerosene. The accompanying gaseous-phase thermodynamics of the surrogate fuel is anchored with the heat of formation of kerosene and verified by comparing a series of one-dimensional rocket thrust chamber calculations. The quasi-global combustion kinetics model consists of several global steps for parent fuel decomposition, soot formation, and soot oxidation and a detailed wet-CO mechanism to complete the combustion process. The final thermophysics formulations are incorporated with a computational fluid dynamics model for prediction of the combustion efficiency of an unielement, tripropellant combustor and the radiation of a kerosene-fueled thruster plume. The model predictions agreed reasonably well with those of the tests.

Process for non-contact removal of organic coatings from the surface of paintings

NASA Technical Reports Server (NTRS)

Banks, Bruce A. (Inventor); Rutledge, Sharon K. (Inventor)

1995-01-01

The present invention discloses a method of removing organic protective coatings from a painting. In the present invention degraded protective coatings such as lacquers, acrylics, natural resins, carbons, soot, and polyurethane are safely removed from the surface of a painting without contact to the surface of the painting. This method can be used for restoration of paintings when they have been damaged, through age, fire, etc.

Flexible conformable hydrophobized surfaces for turbulent flow drag reduction

PubMed Central

Brennan, Joseph C; Geraldi, Nicasio R; Morris, Robert H; Fairhurst, David J; McHale, Glen; Newton, Michael I

2015-01-01

In recent years extensive work has been focused onto using superhydrophobic surfaces for drag reduction applications. Superhydrophobic surfaces retain a gas layer, called a plastron, when submerged underwater in the Cassie-Baxter state with water in contact with the tops of surface roughness features. In this state the plastron allows slip to occur across the surface which results in a drag reduction. In this work we report flexible and relatively large area superhydrophobic surfaces produced using two different methods: Large roughness features were created by electrodeposition on copper meshes; Small roughness features were created by embedding carbon nanoparticles (soot) into Polydimethylsiloxane (PDMS). Both samples were made into cylinders with a diameter under 12 mm. To characterize the samples, scanning electron microscope (SEM) images and confocal microscope images were taken. The confocal microscope images were taken with each sample submerged in water to show the extent of the plastron. The hydrophobized electrodeposited copper mesh cylinders showed drag reductions of up to 32% when comparing the superhydrophobic state with a wetted out state. The soot covered cylinders achieved a 30% drag reduction when comparing the superhydrophobic state to a plain cylinder. These results were obtained for turbulent flows with Reynolds numbers 10,000 to 32,500. PMID:25975704

Morphology of diesel soot residuals from supercooled water droplets and ice crystals: Implications for optical properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

China, Swarup; Kulkarni, Gourihar; Scarnato, Barbara V.

Freshly emitted soot particles are fractal-like aggregates, but atmospheric processing often transforms their morphology. Morphology of soot particles plays an important role in determining their optical properties, life cycle and hence their effect on Earth’s radiative balance. However, little is known about the morphology of soot particles that participated in cold cloud processes. Here we report results from laboratory experiments that simulate cold cloud processing of diesel soot particles by allowing them to form supercooled droplets and ice crystals at -20 and -40°C, respectively. Electron microscopy revealed that soot residuals from ice crystals were more compact (roundness~0.55) than those frommore » supercooled droplets (roundness ~0.45), while nascent soot particles were the least compact (roundness~0.41). Optical simulations using the discrete dipole approximation showed that the more compact structure enhances soot single scattering albedo by a factor up to 1.4, thereby reducing the top-of-the-atmosphere direct radiative forcing by ~63%. Lastly, these results underscore that climate models should consider the morphological evolution of soot particles due to cold cloud processing to improve the estimate of direct radiative forcing of soot.« less

Morphology of diesel soot residuals from supercooled water droplets and ice crystals: Implications for optical properties

DOE PAGES

China, Swarup; Kulkarni, Gourihar; Scarnato, Barbara V.; ...

2015-11-01

Freshly emitted soot particles are fractal-like aggregates, but atmospheric processing often transforms their morphology. Morphology of soot particles plays an important role in determining their optical properties, life cycle and hence their effect on Earth’s radiative balance. However, little is known about the morphology of soot particles that participated in cold cloud processes. Here we report results from laboratory experiments that simulate cold cloud processing of diesel soot particles by allowing them to form supercooled droplets and ice crystals at -20 and -40°C, respectively. Electron microscopy revealed that soot residuals from ice crystals were more compact (roundness~0.55) than those frommore » supercooled droplets (roundness ~0.45), while nascent soot particles were the least compact (roundness~0.41). Optical simulations using the discrete dipole approximation showed that the more compact structure enhances soot single scattering albedo by a factor up to 1.4, thereby reducing the top-of-the-atmosphere direct radiative forcing by ~63%. Lastly, these results underscore that climate models should consider the morphological evolution of soot particles due to cold cloud processing to improve the estimate of direct radiative forcing of soot.« less

Ignition and early soot formation in a DI diesel engine using multiple 2-D imaging diagnostics

NASA Astrophysics Data System (ADS)

Dec, John E.; Espey, Christoph

Combined optical imaging diagnostics in the fuel jet of a direct-injection diesel engine to study the ignition and early soot formation processes. A diesel engine of the 'heavy-duty' size class was operated at a representative medium speed (1200 rpm) operating condition. Two fuels were used, a 42.5 cetane number mixture of the diesel reference fuels and a new low-sooting fuel. Combustion and soot formation are almost identical for both fuels. Ignition and early combustion were studied by imaging the natural chemiluminescence using a calibrated intensified video camera. Early soot development was investigated via luminosity imaging and simultaneous planar imaging of laser-induced incandescence (LII) and elastic scattering. The latter provide relative soot concentrations and particle size distributions. Data show that ignition occurs at multiple points across the downstream region of all the fuel jets prior to first apparent heat release well before any soot luminosity occurs. Quantitative vapor-fuel/air mixture images in the leading portion of the jet are also presented and discussed with respect to the early combustion data. The first soot occurs at random locations, and shortly thereafter, small soot particles develop throughout the cross section of the leading portion of the jet. Data indicate that this soot arises from the fuel-rich premixed burn. Then, significantly larger soot particles appear around the periphery of the jet, presumably from the initial diffusion combustion. By the end of the premixed burn, the soot has developed a distribution pattern of a higher concentration toward the front of the jet and a lower concentration upstream, with the larger-sized soot particles being generally confined to the periphery of the jet.

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

NASA Astrophysics Data System (ADS)

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

2017-04-01

Atmospheric soot particles are primary particles produced by incomplete combustion of biomass and/or fossil fuels. Thus soot mainly originates from anthropogenic emissions, stemming from combustion related processes in transport vehicles, industrial and residential uses. Such soot particles are generally complex mixtures of black carbon (BC) and organic matter (OM) (Bond et al., 2013; Petzold et al., 2013), depending on the sources and the interaction of the primary particles with other atmospheric matter and/or gases BC absorbs solar radiation having a warming effect on global climate. It can also act as a heterogeneous ice nucleating particle (INP) and thus impact cloud-radiation interactions, potentially cooling the climate (Lohmann, 2002). Previous studies, however, have shown conflicting results concerning the ice nucleation ability of soot, limiting the ability to predict its effects on Earth's radiation budget. Here we present a laboratory study where we systematically investigate the ice nucleation behavior of different soot particles. Commercial soot samples are used, including an amorphous, industrial carbon frequently used in coatings and coloring (FW 200, Orion Engineered Carbons) and a fullerene soot (572497 ALDRICH), e.g. used as catalyst. In addition, we use soot generated from a propane flame Combustion Aerosol Standard Generator (miniCAST, JING AG), as a proxy for atmospheric soot particles. The ice nucleation ability of these soot types is tested on size-selected particles for a wide temperature range from 253 K to 218 K, using the Horizontal Ice Nucleation Chamber (HINC), a Continuous Flow Diffusion Chamber (CFDC) (Kanji and Abbatt, 2009). Ice nucleation results from these soot surrogates will be compared to chemically more complex real world samples, collected on filters. Filters will be collected during the 2016/2017 winter haze periods in Beijing, China and represent atmospheric soot particles with sources from both industrial and residential 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.

Quantifying uncertainty in soot volume fraction estimates using Bayesian inference of auto-correlated laser-induced incandescence measurements

NASA Astrophysics Data System (ADS)

Hadwin, Paul J.; Sipkens, T. A.; Thomson, K. A.; Liu, F.; Daun, K. J.

2016-01-01

Auto-correlated laser-induced incandescence (AC-LII) infers the soot volume fraction (SVF) of soot particles by comparing the spectral incandescence from laser-energized particles to the pyrometrically inferred peak soot temperature. This calculation requires detailed knowledge of model parameters such as the absorption function of soot, which may vary with combustion chemistry, soot age, and the internal structure of the soot. This work presents a Bayesian methodology to quantify such uncertainties. This technique treats the additional "nuisance" model parameters, including the soot absorption function, as stochastic variables and incorporates the current state of knowledge of these parameters into the inference process through maximum entropy priors. While standard AC-LII analysis provides a point estimate of the SVF, Bayesian techniques infer the posterior probability density, which will allow scientists and engineers to better assess the reliability of AC-LII inferred SVFs in the context of environmental regulations and competing diagnostics.

Laminar Diffusion Flame Studies (Ground- and Space-Based Studies)

NASA Technical Reports Server (NTRS)

Dai, Z.; El-Leathy, A. M.; Lin, K.-C.; Sunderland, P. B.; Xu, F.; Faeth, G. M.; Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2000-01-01

Laminar diffusion flames are of interest because they provide model flame systems that are far more tractable for analysis and experiments than more practical turbulent diffusion flames. Certainly, understanding flame processes within laminar diffusion flames must precede understanding these processes in more complex turbulent diffusion flames. In addition, many properties of laminar diffusion flames are directly relevant to turbulent diffusion flames using laminar flamelet concepts. Laminar jet diffusion flame shapes (luminous flame boundaries) have been of particular interest since the classical study of Burke and Schumann because they are a simple nonintrusive measurement that is convenient for evaluating flame structure predictions. Thus, consideration of laminar flame shapes is undertaken in the following, emphasizing conditions where effects of gravity are small, due to the importance of such conditions to practical applications. Another class of interesting properties of laminar diffusion flames are their laminar soot and smoke point properties (i.e., the flame length, fuel flow rate, characteristic residence time, etc., at the onset of soot appearance in the flame (the soot point) and the onset of soot emissions from the flame (the smoke point)). These are useful observable soot properties of nonpremixed flames because they provide a convenient means to rate several aspects of flame sooting properties: the relative propensity of various fuels to produce soot in flames; the relative effects of fuel structure, fuel dilution, flame temperature and ambient pressure on the soot appearance and emission properties of flames; the relative levels of continuum radiation from soot in flames; and effects of the intrusion of gravity (or buoyant motion) on emissions of soot from flames. An important motivation to define conditions for soot emissions is that observations of laminar jet diffusion flames in critical environments, e.g., space shuttle and space station facilities, cannot involve soot emitting flames in order to ensure that test chamber windows used for experimental observations are not blocked by soot deposits, thereby compromising unusually valuable experimental results. Another important motivation to define conditions where soot is present in diffusion flames is that flame chemistry, transport and radiation properties are vastly simplified when soot is absent, making such flames far more tractable for detailed numerical simulations than corresponding soot-containing flames. Motivated by these observations, the objectives of this phase of the investigation were as follows: (1) Observe flame-sheet shapes (the location of the reaction zone near phi=1) of nonluminous (soot free) laminar jet diffusion flames in both still and coflowing air and use these results to develop simplified models of flame-sheet shapes for these conditions; (2) Observe luminous flame boundaries of luminous (soot-containing) laminar jet diffusion flames in both still and coflowing air and use these results to develop simplified models of luminous flame boundaries for these conditions. In order to fix ideas here, maximum luminous flame boundaries at the laminar smoke point conditions were sought, i.e., luminous flame boundaries at the laminar smoke point; (3) Observe effects of coflow on laminar soot- and smoke-point conditions because coflow has been proposed as a means to control soot emissions and minimize the presence of soot in diffusion flames.

Soot and palynologic analysis of Manson impact-related strata (Upper Cretaceous) of Iowa and South Dakota, USA

USGS Publications Warehouse

Varricchio, D.J.; Raven, R.F.; Wolbach, W.S.; Elsik, W.C.; Witzke, B.J.

2009-01-01

The Campanian Manson impact structure of Iowa represents the best-preserved, large-diameter complex crater within the continental U.S. To assess the timing and potential mode of crater infilling and the possible presence of an impact event horizon, we analyzed samples from both within and distal to the impact structure for their elemental carbon, soot and palynomorphs. Within the impact structure, identifiable soot occurred in fragmented impact breccia and suevite but not in lower impact-melt breccia. Although most of this soot likely represents reworking of material from older Cretaceous marine shales, one high soot concentration occurs with melt material in a Keweenawan Shale-Phanerozoic clast breccia mix. This represents the first association of soot and impact-generated materials within an impact structure and the best sample candidate for Manson impact-generated soot. No palynomorphs occurred in the impact melt breccia. Overlying suevite (Keweenawan Shale clast breccia) of the central peak yielded sparse and thermally altered palynomorphs, indicating deposition prior to full cooling of the crater debris. Presence of easily degraded soot also argues for rapid backfilling of the crater. Distal samples from South Dakota represent the Sharon Springs and Crow Creek members of the Pierre Shale 230 km northwest of the Manson impact structure. Although containing shocked grains, the Crow Creek preserves no soot. In contrast, the Sharon Springs, generally considered as predating the Manson impact, has significant soot quantities. Palynomorphs differ markedly across the unconformity separating the two members with the Crow Creek containing more terrestrial forms, normapolles, and older reworked palynomorphs, consistent with a terrestrial impact to the east. Origin of the Sharon Springs soot remains unclear. Given soot occurrence within four of the five Cretaceous marine units sampled, the relatively shallow, anoxic bottom conditions of the Western Interior Cretaceous Seaway may have simply favored soot preservation. Until a better understanding of the broader occurrence and preservation of soot is achieved, some soot-impact associations will remain ambiguous. ?? 2008 Elsevier Ltd. All rights reserved.

Preparation and Testing of Corrosion-and Spallation-Resistant Coatings

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hurley, John

2013-10-31

This Energy & Environmental Research Center (EERC) project is designed to determine if plating APMT®, a specific highly oxidation-resistant oxide dispersion-strengthened FeCrAl alloy made by Kanthal, onto nickel-based superalloy turbine parts is a viable method for substantially improving the lifetimes and maximum use temperatures of the parts. The method for joining the APMT plate to the superalloys is called evaporative metal bonding and involves placing a thin foil of zinc (Zn) between the plate and the superalloy, clamping them together, and heating in an atmosphere-controlled furnace. Upon heating, the Zn melts and dissolves the oxide skins of the alloys atmore » the bond line, allowing the two alloys to diffuse into each other. The Zn then diffuses through the alloys and evaporates from their surfaces. Laboratory testing to determine the diffusion rate of Zn through the alloys has been completed. We have found that we were not able to create joints when temperatures much lower than the original temperature of 1214°C are used. Therefore, we limited our diffusion rate measurements to the two hold temperatures used in the procedure: 700° and 1214°C. The diffusivity of zinc in both APMT and CM247LC is quite similar at 700°C. Diffusivity in the APMT appears to be slightly higher, but the midline composition after 30 minutes at this temperature is quite similar. At 1214°C, the situation is very different. The calculated diffusivity of zinc in APMT is approximately 15 times higher than in CM247LC or Rene® 80 (~120 vs. ~8 μm²/min) at that temperature. In addition to the diffusion work, the coefficients of thermal expansions were determined for each of the alloys as a function of temperature. This information has been entered into a finite element model using ANSYS so that appropriate force-applying structures can be designed for use in joining structures composed of APMT and the nickel alloys. Gasifier sampling activities continue to determine what types of trace contaminants may occur in cleaned syngas that could lead to corrosion or deposition in turbines firing coal syngas. The EERC has several pilot-scale gasifiers that are continually used in a variety of test configurations as determined by the needs of the projects that are funding the tests. We are sampling both noncombusted and combusted syngas produced during some of the pilot-scale gasifier tests. After modifying our sampling procedures to minimize contamination from the oxidizer, we obtained very good filter samples from both syngas and from the combustion products of the syngas blended with natural gas. Scanning electron microscopy analyses showed that the particles captured on the filter from the syngas were typically 0.2 to 0.5 μm in diameter, whereas those captured from the combusted syngas were slightly larger and more spherical. However, the particles were so small that we could not obtain good spectra from them either at the EERC or JEOL America, the maker of the EERC electron microscope systems. Therefore, the EERC applied for and received time on electron microscopes using different signal analyzers at the Oak Ridge National Laboratory (ORNL) ShaRE User Facility, which is sponsored by the U.S. Department of Energy Scientific User Facilities Division of the Office of Basic Energy Sciences. At ORNL, both x-ray photoelectron spectroscopy (XPS) and Auger electron spectroscopy were performed on the samples because these are surface analyses that analyze electrons emitted from within a few nanometers of the surfaces of the particles and filters. The XPS data show that the particles do not contain any metals and, in fact, have an atomic composition almost identical to that of the polycarbonate filter. We currently believe that this indicates that the particles are primarily soot-based and not formed from volatilization of metals in the fluid-bed gasifier. The data indicate that the soot-based particles are not well burned in the thermal oxidizer, although they are significantly oxidized, nitrided, and sulfidized in the combustor. Ion etching to remove the surfaces of the particles indicates that the oxidation, nitridation, and sulfidation of the particles are primarily surface phenomena.« less

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

PubMed

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

PubMed Central

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

Acoustic filtration and sedimentation of soot particles

NASA Astrophysics Data System (ADS)

Martin, K. M.; Ezekoye, O. A.

Removal of soot particles from a static chamber by an intense acoustic field is investigated. Combustion of a solid fuel fills a rectangular chamber with small soot particles, which sediment very slowly. The chamber is then irradiated by an intense acoustic source to produce a three dimensional standing wave field in the chamber. The acoustic excitation causes the soot particles to agglomerate, forming larger particles which sediment faster from the system. The soot also forms 1-2 cm disks, with axes parallel to the axis of the acoustic source, which are levitated by the sound field at half-wavelength spacing within the chamber. Laser extinction measurements are made to determine soot volume fractions as a function of exposure time within the chamber. The volume fraction is reduced over time by sedimentation and by particle migration to the disks. The soot disks are considered to be a novel mechanism for particle removal from the air stream, and this mechanism has been dubbed acoustic filtration. An experimental method is developed for comparing the rate of soot removal by sedimentation alone with the rate of soot removal by sedimentation and acoustic filtration. Results show that acoustic filtration increases the rate of soot removal by a factor of two over acoustically-induced sedimentation alone.

Characterization of soot properties in two-meter JP-8 pool fires.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Suo-Anttila, Jill Marie; Jensen, Kirk A.; Blevins, Linda Gail

2005-02-01

The thermal hazard posed by large hydrocarbon fires is dominated by the radiative emission from high temperature soot. Since the optical properties of soot, especially in the infrared region of the electromagnetic spectrum, as well as its morphological properties, are not well known, efforts are underway to characterize these properties. Measurements of these soot properties in large fires are important for heat transfer calculations, for interpretation of laser-based diagnostics, and for developing soot property models for fire field models. This research uses extractive measurement diagnostics to characterize soot optical properties, morphology, and composition in 2 m pool fires. For measurementmore » of the extinction coefficient, soot extracted from the flame zone is transported to a transmission cell where measurements are made using both visible and infrared lasers. Soot morphological properties are obtained by analysis via transmission electron microscopy of soot samples obtained thermophoretically within the flame zone, in the overfire region, and in the transmission cell. Soot composition, including carbon-to-hydrogen ratio and polycyclic aromatic hydrocarbon concentration, is obtained by analysis of soot collected on filters. Average dimensionless extinction coefficients of 8.4 {+-} 1.2 at 635 nm and 8.7 {+-} 1.1 at 1310 nm agree well with recent measurements in the overfire region of JP-8 and other fuels in lab-scale burners and fires. Average soot primary particle diameters, radius of gyration, and fractal dimensions agree with these recent studies. Rayleigh-Debye-Gans theory of scattering applied to the measured fractal parameters shows qualitative agreement with the trends in measured dimensionless extinction coefficients. Results of the density and chemistry are detailed in the report.« less

Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

NASA Astrophysics Data System (ADS)

Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

2014-12-01

Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Hai; Kook, Sanghoon; Doom, Jeffrey

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 surrogatemore » 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 model to accurately predict gas temperatures and thus soot formation rates. When including such a radiation model, the LES model predicts mean soot concentrations within 30% in the ethylene jet flame.« less

Optical investigation of the combustion behaviour inside the engine operating in HCCI mode and using alternative diesel fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mancaruso, E.; Vaglieco, B.M.

2010-04-15

In order to understand the effect of both the new homogeneous charge compression ignition (HCCI) combustion process and the use of biofuel, optical measurements were carried out into a transparent CR diesel engine. Rape seed methyl ester was used and tests with several injection pressures were performed. OH and HCO radical were detected and their evolutions were analyzed during the whole combustion. Moreover, soot concentration was measured by means the two colour pyrometry method. The reduction of particulate emission with biodiesel as compared to the diesel fuel was noted. Moreover, this effect resulted higher increasing the injection pressure. In themore » case of RME the oxidation of soot depends mainly from O{sub 2} content of fuel and OH is responsible of the NO formation in the chamber as it was observed for NO{sub x} exhaust emission. Moreover, it was investigated the evolution of HCO and CO into the cylinder. HCO was detected at the start of combustion. During the combustion, HCO oxidizes due to the increasing temperature and it produces CO. Both fuels have similar trend, the highest concentrations are detected for low injection pressure. This effect is more evident for the RME fuel. (author)« less

X-ray scattering and spectroscopy studies on diesel soot from oxygenated fuel under various engine load conditions

USGS Publications Warehouse

Braun, Andreas; Shah, N.; Huggins, Frank E.; Kelly, K.E.; Sarofim, A.; Jacobsen, C.; Wirick, S.; Francis, H.; Ilavsky, J.; Thomas, G.E.; Huffman, G.P.

2005-01-01

Diesel soot from reference diesel fuel and oxygenated fuel under idle and load engine conditions was investigated with X-ray scattering and X-ray carbon K-edge absorption spectroscopy. Up to five characteristic size ranges were found. Idle soot was generally found to have larger primary particles and aggregates but smaller crystallites, than load soot. Load soot has a higher degree of crystallinity than idle soot. Adding oxygenates to diesel fuel enhanced differences in the characteristics of diesel soot, or even reversed them. Aromaticity of idle soot from oxygenated diesel fuel was significantly larger than from the corresponding load soot. Carbon near-edge X-ray absorption fine structure (NEXAFS) spectroscopy was applied to gather information about the presence of relative amounts of carbon double bonds (CC, CO) and carbon single bonds (C-H, C-OH, COOH). Using scanning X-ray transmission microspectroscopy (STXM), the relative amounts of these carbon bond states were shown to vary spatially over distances approximately 50 to 100 nm. The results from the X-ray techniques are supported by thermo-gravimetry analysis and high-resolution transmission electron microscopy. ?? 2005 Elsevier Ltd. All rights reserved.

Effect of traffic and driving characteristics on morphology of atmospheric soot particles at freeway on-ramps.

PubMed

China, Swarup; Salvadori, Neila; Mazzoleni, Claudio

2014-03-18

Vehicles represent a major source of soot in urban environments. Knowledge of the morphology and mixing of soot particles is fundamental to understand their potential health and climatic impacts. We investigate 5738 single particles collected at six different cloverleaf freeway on-ramps in Southern Michigan, using 2D images from scanning electron microscopy. Of those, 3364 particles are soot. We present an analysis of the morphological and mixing properties of those soot particles. The relative abundance of soot particles shows a positive association with traffic density (number of vehicles per minute). A classification of the mixing state of freshly emitted soot particles shows that most of them are bare (or thinly coated) (72%) and some are partly coated (22%). We find that the fractal dimension of soot particles (one of the most relevant morphological descriptors) varies from site to site, and increases with increasing vehicle specific power that represents the driving/engine load conditions, and with increasing percentage of vehicles older than 15 years. Our results suggest that driving conditions, and vehicle age and type have significant influence on the morphology of soot particles.

Scattering and radiative properties of complex soot and soot-containing particles

NASA Astrophysics Data System (ADS)

Liu, L.; Mishchenko, M. I.; Mackowski, D. W.; Dlugach, J.

2012-12-01

Tropospheric soot and soot containing aerosols often exhibit nonspherical overall shapes and complex morphologies. They can externally, semi-externally, and internally mix with other aerosol species. This poses a tremendous challenge in particle characterization, remote sensing, and global climate modeling studies. To address these challenges, we used the new numerically exact public-domain Fortran-90 code based on the superposition T-matrix method (STMM) and other theoretical models to analyze the potential effects of aggregation and heterogeneity on light scattering and absorption by morphologically complex soot containing particles. The parameters we computed include the whole scattering matrix elements, linear depolarization ratios, optical cross-sections, asymmetry parameters, and single scattering albedos. It is shown that the optical characteristics of soot and soot containing aerosols very much depend on particle sizes, compositions, and aerosol overall shapes. The soot particle configurations and heterogeneities can have a substantial effect that can result in a significant enhancement of extinction and absorption relative to those computed from the Lorenz-Mie theory. Meanwhile the model calculated information combined with in-situ and remote sensed data can be used to constrain soot particle shapes and sizes which are much needed in climate models.

Fuel Preheat Effects on Soot-Field Structure in Laminar Gas Jet Diffusion Flames Burning in 0-g and 1-g

NASA Technical Reports Server (NTRS)

Konsur, Bogdan; Megaridis, Constantine M.; Griffin, Devon W.

1999-01-01

An experimental investigation conducted at the 2.2-s drop tower of the NASA Lewis Research Center is presented to quantify the influence of moderate fuel preheat on soot-field structure within 0-g laminar gas jet diffusion flames. Parallel work in 1-g is also presented to delineate the effect of elevated fuel temperatures on soot-field structure in buoyant flames. The experimental methodology implements jet diffusion flames of nitrogen-diluted acetylene fuel burning in quiescent air at atmospheric pressure. Fuel preheat of approximately 100 K in the 0-g laminar jet diffusion flames is found to reduce soot loadings in the annular region, but causes an increase in soot volume fractions at the centerline. In addition, fuel preheat reduces the radial extent of the soot field in 0-g. In 1-g, the same fuel preheat levels have a more moderated influence on soot loadings in the annular region, but are also seen to enhance soot concentrations near the axis low in the flame. The increased soot loadings near the flame centerline, as caused by fuel preheat, are consistent with the hypothesis that preheat levels of approximately 100 K enhance fuel pyrolysis rates. The results show that the growth stage of particles transported along the soot annulus is shortened both in 1-g and 0-g when elevated fuel temperatures are used.

Soot Formation in Freely-Propagating Laminar Premixed Flames

NASA Technical Reports Server (NTRS)

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.

Mixed-phase aerosol particles

NASA Astrophysics Data System (ADS)

Corti, T.; Krieger, U. K.; Koop, T.; Peter, T.

2003-04-01

Within a liquid aerosol particle a solid phase may coexist with the liquid over a wide range of ambient conditions. The optical properties of such particles are of interest for a number of reasons. They will affect the scattering albedo of atmospheric aerosols, may cause depolarisation in lidar measurements, and potentially open a window for studying the internal morphology and physical properties (e.g. wetting properties, diffusion constants) of composite particles in laboratory experiments. In this contribution, we will present results of experimental and theoretical work on mixed-phase aerosol particles. The optical properties of mixed-phase particles depend on the location of the inclusion in the liquid phase, which is determined by the surface tensions of the involved interfaces. In the case of complete wetting, the energetically favoured position of the inclusion is in the volume of the liquid phase. For partial wetting, a position at the surface of the liquid phase is favoured, with the contact angle between the solid, liquid and air being described by Young's equation. For systems with small contact angles, the difference in energy between an inclusion situated at the droplets surface and in its volume may be so small that the thermal energy kT is sufficient to displace the inclusion from the droplet surface into its volume. The critical contact angle depends on the size of the inclusion and the droplet and ranges from 0.1 to 10 degrees. Examples of mixed-phase aerosol particles are aged soot particles and sea salt particles at low relative humidity. For aged soot, contact angles on sulphuric acid clearly above 10 degrees have been reported, so that soot inclusions are expected to be located at the surface of aerosol particles. For mixed-phase sea salt particles, consisting of a solid NaCl inclusion and an aqueous solution of mainly NaCl and MgCl2, our measurements on macroscopic NaCl crystals show a contact angle clearly below 10 degrees and possibly as low as 0.1 degrees. An experimental method - based on measuring photon count statistics - is developed to distinguish in single levitated aerosol particle whether a solid inclusion is located in the volume of the particle or at its surface.

Military Housing Inspections - Republic of Korea

DTIC Science & Technology

2014-10-28

Soot build-up on surfaces and around vent flue joints and dampers of the boilers in the mechanical rooms were signs of inadequate combustion...Illuminated sensor probe indicates that conductor is energized (Deficiency No. YON‑EL‑140310‑015) Source: DoD OIG Disconnected Ground Wire Installation

The effect of mineral dust and soot aerosols on ice microphysics near the foothills of the Himalayas: A numerical investigation

NASA Astrophysics Data System (ADS)

Hazra, Anupam; Padmakumari, B.; Maheskumar, R. S.; Chen, Jen-Ping

2016-05-01

This study investigates the influence of different ice nuclei (IN) species and their number concentrations on cloud ice production. The numerical simulation with different species of ice nuclei is investigated using an explicit bulk-water microphysical scheme in a Mesoscale Meteorological Model version 5 (MM5). The species dependent ice nucleation parameterization that is based on the classical nucleation theory has been implemented into the model. The IN species considered include dust and soot with two different concentrations (Low and High). The simulated cloud microphysical properties like droplet number concentration and droplet effective radii as well as macro-properties (equivalent potential temperature and relative humidity) are comparable with aircraft observations. When higher dust IN concentrations are considered, the simulation results showed good agreement with the cloud ice and cloud water mixing ratio from aircraft measurements during Cloud Aerosol Interactions and Precipitation Enhancement Experiment (CAIPEEX) and Modern Era Retrospective Analysis for Research and Applications (MERRA) reanalysis. Relative importance of IN species is shown as compared to the homogeneous freezing nucleation process. The tendency of cloud ice production rates is also analyzed and found that dust IN is more efficient in producing cloud ice when compared to soot IN. The dust IN with high concentration can produce more surface precipitation than soot IN at the same concentration. This study highlights the need to improve the ice nucleation parameterization in numerical models.

An experimental study of high-pressure droplet combustion

NASA Technical Reports Server (NTRS)

Norton, Chris M.; Litchford, Ron J.; Jeng, San-Mou

1990-01-01

The results are presented of an experimental study on suspended n-heptane droplet combustion in air for reduced pressures up to P(r) = 2.305. Transition to fully transient heat-up through the critical state is demonstrated above a threshold pressure corresponding to P(r) of roughly 1.4. A silhouette imaging technique resolves the droplet surface for reduced pressures up to about P(r) roughly 0.63, but soot formation conceals the surface at higher pressures. Images of the soot plumes do not show any sudden change in behavior indicative of critical transition. Mean burning rate constants are computed from the d-squared variation law using measured effective droplet diameters at ignition and measured burn times, and corrected burning times are computed for an effective initial droplet diameter. The results show that the burning rates increase as the fuel critical pressure is approached and decrease as the pressure exceeds the fuel critical pressure. Corrected burning times show inverse behavior.

Laser-induced incandescence calibration via gravimetric sampling

NASA Technical Reports Server (NTRS)

Choi, M. Y.; Vander Wal, R. L.; Zhou, Z.

1996-01-01

Absolute calibration of laser-induced incandescence (LII) is demonstrated via comparison of LII signal intensities with gravimetrically determined soot volume fractions. This calibration technique does not rely upon calculated or measured optical characteristics of soot. The variation of the LII signal with gravimetrically measured soot volume fractions ranging from 0.078 to 1.1 ppm established the linearly of the calibration. With the high spatial and temporal resolution capabilities of laser-induced incandescence (LII), the spatial and temporal fluctuations of the soot field within a gravimetric chimney were characterized. Radial uniformity of the soot volume fraction, f(sub v) was demonstrated with sufficient averaging of the single laser-shot LII images of the soot field thus confirming the validity of the calibration method for imaging applications. As illustration, instantaneous soot volume fractions within a Re = 5000 ethylene/air diffusion flame measured via planar LII were established quantitatively with this calibration.

Conductometric Sensor for Soot Mass Flow Detection in Exhausts of Internal Combustion Engines

PubMed Central

Feulner, Markus; Hagen, Gunter; Müller, Andreas; Schott, Andreas; Zöllner, Christian; Brüggemann, Dieter; Moos, Ralf

2015-01-01

Soot sensors are required for on-board diagnostics (OBD) of automotive diesel particulate filters (DPF) to detect filter failures. Widely used for this purpose are conductometric sensors, measuring an electrical current or resistance between two electrodes. Soot particles deposit on the electrodes, which leads to an increase in current or decrease in resistance. If installed upstream of a DPF, the “engine-out” soot emissions can also be determined directly by soot sensors. Sensors were characterized in diesel engine real exhausts under varying operation conditions and with two different kinds of diesel fuel. The sensor signal was correlated to the actual soot mass and particle number, measured with an SMPS. Sensor data and soot analytics (SMPS) agreed very well, an impressing linear correlation in a double logarithmic representation was found. This behavior was even independent of the used engine settings or of the biodiesel content. PMID:26580621

Conductometric Sensor for Soot Mass Flow Detection in Exhausts of Internal Combustion Engines.

PubMed

Feulner, Markus; Hagen, Gunter; Müller, Andreas; Schott, Andreas; Zöllner, Christian; Brüggemann, Dieter; Moos, Ralf

2015-11-13

Soot sensors are required for on-board diagnostics (OBD) of automotive diesel particulate filters (DPF) to detect filter failures. Widely used for this purpose are conductometric sensors, measuring an electrical current or resistance between two electrodes. Soot particles deposit on the electrodes, which leads to an increase in current or decrease in resistance. If installed upstream of a DPF, the "engine-out" soot emissions can also be determined directly by soot sensors. Sensors were characterized in diesel engine real exhausts under varying operation conditions and with two different kinds of diesel fuel. The sensor signal was correlated to the actual soot mass and particle number, measured with an SMPS. Sensor data and soot analytics (SMPS) agreed very well, an impressing linear correlation in a double logarithmic representation was found. This behavior was even independent of the used engine settings or of the biodiesel content.

Particulate Matter from Both Heavy Fuel Oil and Diesel Fuel Shipping Emissions Show Strong Biological Effects on Human Lung Cells at Realistic and Comparable In Vitro Exposure Conditions

PubMed Central

Dilger, Marco; Paur, Hanns-Rudolf; Schlager, Christoph; Mülhopt, Sonja; Diabaté, Silvia; Weiss, Carsten; Stengel, Benjamin; Rabe, Rom; Harndorf, Horst; Torvela, Tiina; Jokiniemi, Jorma K.; Hirvonen, Maija-Riitta; Schmidt-Weber, Carsten; Traidl-Hoffmann, Claudia; BéruBé, Kelly A.; Wlodarczyk, Anna J.; Prytherch, Zoë; Michalke, Bernhard; Krebs, Tobias; Prévôt, André S. H.; Kelbg, Michael; Tiggesbäumker, Josef; Karg, Erwin; Jakobi, Gert; Scholtes, Sorana; Schnelle-Kreis, Jürgen; Lintelmann, Jutta; Matuschek, Georg; Sklorz, Martin; Klingbeil, Sophie; Orasche, Jürgen; Richthammer, Patrick; Müller, Laarnie; Elsasser, Michael; Reda, Ahmed; Gröger, Thomas; Weggler, Benedikt; Schwemer, Theo; Czech, Hendryk; Rüger, Christopher P.; Abbaszade, Gülcin; Radischat, Christian; Hiller, Karsten; Buters, Jeroen T. M.; Dittmar, Gunnar; Zimmermann, Ralf

2015-01-01

Background Ship engine emissions are important with regard to lung and cardiovascular diseases especially in coastal regions worldwide. Known cellular responses to combustion particles include oxidative stress and inflammatory signalling. Objectives To provide a molecular link between the chemical and physical characteristics of ship emission particles and the cellular responses they elicit and to identify potentially harmful fractions in shipping emission aerosols. Methods Through an air-liquid interface exposure system, we exposed human lung cells under realistic in vitro conditions to exhaust fumes from a ship engine running on either common heavy fuel oil (HFO) or cleaner-burning diesel fuel (DF). Advanced chemical analyses of the exhaust aerosols were combined with transcriptional, proteomic and metabolomic profiling including isotope labelling methods to characterise the lung cell responses. Results The HFO emissions contained high concentrations of toxic compounds such as metals and polycyclic aromatic hydrocarbon, and were higher in particle mass. These compounds were lower in DF emissions, which in turn had higher concentrations of elemental carbon (“soot”). Common cellular reactions included cellular stress responses and endocytosis. Reactions to HFO emissions were dominated by oxidative stress and inflammatory responses, whereas DF emissions induced generally a broader biological response than HFO emissions and affected essential cellular pathways such as energy metabolism, protein synthesis, and chromatin modification. Conclusions Despite a lower content of known toxic compounds, combustion particles from the clean shipping fuel DF influenced several essential pathways of lung cell metabolism more strongly than particles from the unrefined fuel HFO. This might be attributable to a higher soot content in DF. Thus the role of diesel soot, which is a known carcinogen in acute air pollution-induced health effects should be further investigated. For the use of HFO and DF we recommend a reduction of carbonaceous soot in the ship emissions by implementation of filtration devices. PMID:26039251

Quantitative characterization of steady and time-varying, sooting, laminar diffusion flames using optical techniques

NASA Astrophysics Data System (ADS)

Connelly, Blair C.

In order to reduce the emission of pollutants such as soot and NO x from combustion systems, a detailed understanding of pollutant formation is required. In addition to environmental concerns, this is important for a fundamental understanding of flame behavior as significant quantities of soot lower local flame temperatures, increase overall flame length and affect the formation of such temperature-dependent species as NOx. This problem is investigated by carrying out coupled computational and experimental studies of steady and time-varying sooting, coflow diffusion flames. Optical diagnostic techniques are a powerful tool for characterizing combustion systems, as they provide a noninvasive method of probing the environment. Laser diagnostic techniques have added advantages, as systems can be probed with high spectral, temporal and spatial resolution, and with species selectivity. Experimental soot volume fractions were determined by using two-dimensional laser-induced incandescence (LII), calibrated with an on-line extinction measurement, and soot pyrometry. Measurements of soot particle size distributions are made using time-resolved LII (TR-LII). Laser-induced fluorescence measurements are made of NO and formaldehyde. These experimental measurements, and others, are compared with computational results in an effort to understand and model soot formation and to examine the coupled relationship of soot and NO x formation.

Reconstruction of atmospheric soot history in inland regions from lake sediments over the past 150 years

PubMed Central

Han, Y. M.; Wei, C.; Huang, R.-J.; Bandowe, B. A. M.; Ho, S. S. H.; Cao, J. J.; Jin, Z. D.; Xu, B. Q.; Gao, S. P.; Tie, X. X.; An, Z. S.; Wilcke, W.

2016-01-01

Historical reconstruction of atmospheric black carbon (BC, in the form of char and soot) is still constrained for inland areas. Here we determined and compared the past 150-yr records of BC and polycyclic aromatic compounds (PACs) in sediments from two representative lakes, Huguangyan (HGY) and Chaohu (CH), in eastern China. HGY only receives atmospheric deposition while CH is influenced by riverine input. BC, char, and soot have similar vertical concentration profiles as PACs in both lakes. Abrupt increases in concentrations and mass accumulation rates (MARs) of soot have mainly occurred since ~1950, the establishment of the People’s Republic of China, when energy usage changed to more fossil fuel contributions reflected by the variations in the concentration ratios of char/soot and individual PACs. In HGY, soot MARs increased by ~7.7 times in the period 1980–2012 relative to the period 1850–1950. Similar increases (~6.7 times) were observed in CH. The increase in soot MARs is also in line with the emission inventory records in the literature and the fact that the submicrometer-sized soot particles can be dispersed regionally. The study provides an alternative method to reconstruct the atmospheric soot history in populated inland areas. PMID:26750586

Microgravity Superagglomerates Produced By Silane And Acetylene

NASA Technical Reports Server (NTRS)

Gokoglu, Suleyman (Technical Monitor); Bundy, Matthew; Mulholland, George W.; Manzello, Samuel; Yang, Jiann; Scott, John Henry; Sivathanu, Yudaya

2003-01-01

The size of the agglomerates produced in the upper portion of a flame is important for a variety of applications. Soot particle size and density effect the amount of radiative heat transfer from a fire to its surroundings. Particle size determines the lifetime of smoke in a building or in the atmosphere, and exposure hazard for smoke inhaled and deposited in the lungs. The visibility through a smoke layer and dectectability of the smoke are also greatly affected by agglomerate size. Currently there is limited understanding of soot growth with an overall dimension of 10 m and larger. In the case of polystyrene, smoke agglomerates in excess of 1 mm have been observed raining out from large fires. Unlike hydrocarbon fuels, silane has the advantage that silica particles are the major combustion product resulting in a particle volume fraction a factor of ten greater than that for a carbonaceous smoke. There are two very desirable properties of silica aero-gels that are important for both space and earth based applications. The first important property is its inertness to most oxidizing and reducing atmospheres. Therefore, silica aero-gels make excellent fire ablatives and can be used in very demanding applications. The second important property is that silica aero-gels are expected to have very high porosity (greater than 0.999), making them lightweight and ideal for aerospace applications. The added benefit of the high porosity is that they can be used as extremely efficient filters for many earth based applications as well. Evidence of the formation of superagglomerates in a laminar acetylene/air diffusion flame was found by Sorensen et al. [1]. An interconnecting web of super-agglomerates was observed to span the width of the soot plume in the region just above the flame tip and described as a gel state. It was observed that this gel state immediately breaks up into agglomerates as larges as 100 m due to buoyancy induced turbulence. Large soot agglomerates were observed in microgravity butane jet diffusion flames by Ito et al.[2]. Several other works to date have studied the effect of flame structure on soot volume fraction and agglomeration size in a microgravity environment.[3-4]. In microgravity the absence of buoyant convective flows increases the residence time in the flame and causes a broadening of the high temperature region in the flame. Both of these factors play a significant role in gas phase radiation and soot formation

Effects of soot absorption coefficient-Planck function correlation on radiative heat transfer in oxygen-enriched propane turbulent diffusion flame

NASA Astrophysics Data System (ADS)

Consalvi, J. L.; Nmira, F.

2016-03-01

The main objective of this article is to quantify the influence of the soot absorption coefficient-Planck function correlation on radiative loss and flame structure in an oxygen-enhanced propane turbulent diffusion flame. Calculations were run with and without accounting for this correlation by using a standard k-ε model and the steady laminar flamelet model (SLF) coupled to a joint Probability Density Function (PDF) of mixture fraction, enthalpy defect, scalar dissipation rate, and soot quantities. The PDF transport equation is solved by using a Stochastic Eulerian Field (SEF) method. The modeling of soot production is carried out by using a flamelet-based semi-empirical acetylene/benzene soot model. Radiative heat transfer is modeled by using a wide band correlated-k model and turbulent radiation interactions (TRI) are accounted for by using the Optically-Thin Fluctuation Approximation (OTFA). Predicted soot volume fraction, radiant wall heat flux distribution and radiant fraction are in good agreement with the available experimental data. Model results show that soot absorption coefficient and Planck function are negatively correlated in the region of intense soot emission. Neglecting this correlation is found to increase significantly the radiative loss leading to a substantial impact on flame structure in terms of mean and rms values of temperature. In addition mean and rms values of soot volume fraction are found to be less sensitive to the correlation than temperature since soot formation occurs mainly in a region where its influence is low.

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

NASA Astrophysics Data System (ADS)

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.

Molecular modelling investigations on the possibility of phenanthrene dimers to be the primary nuclei of soot

NASA Astrophysics Data System (ADS)

Wei, Mingrui; Wu, Sheng; Li, Fan; Zhang, Dongju; Zhang, Tingting; Guo, Guanlun

2017-11-01

Pyrene dimerisation was successfully used to model the beginning of soot nucleation in some simulation models. However, the quantum mechanics (QM) calculations proved that the binding energy of a PAH dimer with three six-member rings was similar to that of a pyrene dimer. Meanwhile, the high concentration of phenanthrene at flame conditions indicated high probability of collisions among them. The small difference of the binding energy and high concentration indicated that PAHs structurally smaller than pyrene also could be involved in soot inception. Hence, binary collisions of phenanthrene were simulated to find out whether phenanthrene dimers can serve as soot primary nuclei or not by using non-equilibrium molecular dynamics (MD). Three temperatures, six collision orientations and 155 initial translational velocities (ITVs) were considered. The results indicated that the number of dimers with lifetime over 10 ps which can serve as soot nuclei decreased from 52 at 1000 K to 17 at 1600 K, and further to 6 at 2400 K, which means that low temperature was more favourable for phenanthrene to form soot nuclei. Meanwhile, no soot nuclei were formed at the high velocity region (HVR), compared to 43 and 9 at low and middle velocity regions (LVR and MVR), respectively, when temperature was 1000 K. Also, no soot nuclei were formed at HVR when the temperature was raised to 1600 K and 2400 K. This indicated that HVR was unfavourable for phenanthrene to form soot nuclei. The results computationally further illustrated that small PAHs such as phenanthrene could serve as soot primary nuclei, since they have similar mole fractions in some flames. This may be useful for future soot simulation models.

On the radiative properties of soot aggregates - Part 2: Effects of coating

NASA Astrophysics Data System (ADS)

Liu, Fengshan; Yon, Jérôme; Bescond, Alexandre

2016-03-01

The effects of weakly absorbing material coating on soot have attracted considerable research attention in recent years due to the significant influence of such coating on soot radiative properties and the large differences predicted by different numerical models. Soot aggregates were first numerically generated using the diffusion limited cluster aggregation algorithm to produce fractal aggregates formed by log-normally distributed polydisperse spherical primary particles in point-touch. These aggregates were then processed by adding a certain amount of primary particle overlapping and necking to simulate the soot morphology observed from transmission electron microscopy images. After this process, a layer of WAM coating of different thicknesses was added to these more realistic soot aggregates. The radiative properties of these coated soot aggregates over the spectral range of 266-1064 nm were calculated by the discrete dipole approximation (DDA) using the spectrally dependent refractive index of soot for four aggregates containing Np=1, 20, 51 and 96 primary particles. The considered coating thicknesses range from 0% (no coating) up to 100% coating in terms of the primary particle diameter. Coating enhances both the particle absorption and scattering cross sections, with much stronger enhancement to the scattering one, as well as the asymmetry factor and the single scattering albedo. The absorption enhancement is stronger in the UV than in the visible and the near infrared. The simple corrections to the Rayleigh-Debye-Gans fractal aggregates theory for uncoated soot aggregates are found not working for coated soot aggregates. The core-shell model significantly overestimates the absorption enhancement by coating in the visible and the near infrared compared to the DDA results of the coated soot particle. Treating an externally coated soot aggregate as an aggregate formed by individually coated primary particles significantly underestimates the absorption enhancement by coating in the visible and the near infrared.

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

PubMed

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 valuable tool for probing enhanced absorption by soot at atmospherically relevant concentrations.

Heterogeneous atmospheric chemistry

NASA Technical Reports Server (NTRS)

Schryer, D. R.

1982-01-01

The present conference on heterogeneous atmospheric chemistry considers such topics concerning clusters, particles and microparticles as common problems in nucleation and growth, chemical kinetics, and catalysis, chemical reactions with aerosols, electron beam studies of natural and anthropogenic microparticles, and structural studies employing molecular beam techniques, as well as such gas-solid interaction topics as photoassisted reactions, catalyzed photolysis, and heterogeneous catalysis. Also discussed are sulfur dioxide absorption, oxidation, and oxidation inhibition in falling drops, sulfur dioxide/water equilibria, the evidence for heterogeneous catalysis in the atmosphere, the importance of heterogeneous processes to tropospheric chemistry, soot-catalyzed atmospheric reactions, and the concentrations and mechanisms of formation of sulfate in the atmospheric boundary layer.

A unique approach to determine the ice nucleating potential of soot-containing aerosol from biomass combustion

NASA Astrophysics Data System (ADS)

Levin, E. J.; McMeeking, G. R.; McCluskey, C.; DeMott, P. J.; Kreidenweis, S. M.

2013-12-01

Ice nucleating particles (INP) play a crucial role in cloud and precipitation development in mixed phase clouds by catalyzing ice formation at temperatures warmer than -36 C. Despite their importance, however, there is still considerable uncertainty as to the sources and chemical nature of INP. Water insoluble particles such as mineral dust and certain biological aerosols have been shown to be efficient ice nuclei, and soot particles have also been suggested as potential INP. Biomass burning, such as wildfires and prescribed burning, is a large contributor to atmospheric soot concentrations, and could therefore be a potentially important source of INP. Both laboratory and field studies have detected enhanced INP concentrations in smoke plumes; however, the chemical composition of these INP is still uncertain as fires emit and loft a complex mixture of aerosol particles. In this work we employ a novel approach to selectively remove soot aerosol from the sample stream to determine the specific contribution of soot to INP concentrations. A number of commonly consumed biomass fuels were burned in the U.S. Forest Service combustion laboratory during the FLAME-4 (Fire Laboratory At Missoula Experiment - 4) study. Number concentrations of INP acting in the condensation and immersion freezing modes and total aerosol greater than 500 nm in diameter (N500) were measured using the Colorado State University Continuous Flow Diffusion Chamber (CFDC). To determine the contribution of soot to INP concentrations, the sample stream was passed through a Single Particle Soot Photometer (SP2; Droplet Measurement Technologies) which employs laser induced incandescence (LII) to detect soot containing particles and total soot mass. During LII, soot containing particles are vaporized and removed from the sample while non-soot containing particles pass through the instrument unaffected. By sampling the exhaust of the SP2 with the CFDC and alternately cycling laser power on and off we were able to estimate the contribution of soot to total INP. Reductions in both N500 and INP were observed when the laser power was on, indicating both the presence of soot in the total aerosol and the INP fraction of these particles. However, considerable variability was observed in the fraction of INP composed of soot-containing particles with a range from ~0 - 70% for the biomass types and combustion conditions examined.

Radiation and Nitric Oxide Formation in Turbulent Non-Premixed Jet Flames

DTIC Science & Technology

2000-08-04

axial coordinate was nor- malized by the stoichiometric flame length . of possible soot-NO interactions and reduces inter- ference with the laser...through the top of the cylinder was small if the height of the axial traverse was 3 to 4 times the stoi- chiometric flame length . The calibration of the...jet Reynolds numbers, Re, stoichiometric flame length , Lstoich, and convective residence times, s. The convective residence time was determined by s

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

ERIC Educational Resources Information Center

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.…

CuCl2 for the isolation of a broad array of endohedral fullerenes containing metallic, metallic carbide, metallic nitride, and metallic oxide clusters, and separation of their structural isomers.

PubMed

Stevenson, Steven; Rottinger, Khristina A

2013-08-19

A typical arc-synthesis generates many types of fullerenes and endohedrals. Resulting soot extracts contain a complex mixture of >50 types of fullerenes, metallofullerenes, and their structural isomers. Prior to application development, novel separation methods are required to fractionate this rich array of metallic, metallic carbide, metallic nitride, and metallic oxide endohedrals, all of which can be present in a single, soot extract. Herein, we report the discovery of CuCl2 as a Lewis acid that will selectively precipitate only the more reactive members of each of these endohedral families. The more reactive Sc4O2@Ih-C80, Sc3C2@Ih-C80, and Sc3N@D3h-C78 endohedrals are quickly removed from extracts to greatly decrease the number of endohedrals present in a sample. Experiments indicate that enrichment factors of several orders of magnitude can be achieved within minutes of reaction time. CuCl2 also has sufficient selectivity to resolve and separate structural isomers, as demonstrated with Er2@C82 (isomer I, Cs(6)-C82 versus isomer III). The selective complexation of CuCl2 with fullerenes can be correlated to their first oxidation potential. We estimate a significantly lower threshold of precipitation for CuCl2 (<0.19 V) compared to stronger Lewis acids. Fullerenes and metallofullerenes having first oxidation potentials above 0.19 V tend to remain unreacted in solution. In contrast, species with first oxidation potentials below 0.19 V (vs Fc/Fc(+)) precipitate via complexation, and are easily decomplexed. CuCl2 is compared to Lewis acids having higher precipitation thresholds (e.g., FeCl3) in our goal to predict a priori which endohedrals would remain in solution versus which endohedral species would complex and precipitate. The ability to predict endohedral precipitation a priori is beneficial to the design of purification strategies for metallofullerenes.

Leaner Lifted-Flame Combustion Enabled by the Use of an Oxygenated Fuel in an Optical CI Engine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gehmlich, Ryan K.; Dumitrescu, Cosmin E.; Wang, Yefu

Leaner lifted-flame combustion (LLFC) is a mixing-controlled combustion strategy for compression-ignition engines that does not produce soot because the equivalence ratio at the lift-off length, Φ(H), is less than or equal to approximately two. In addition to preventing soot formation, LLFC can simultaneously control emissions of nitrogen oxides because it is tolerant to the use of exhaust-gas recirculation for lowering in-cylinder temperatures. LLFC can be achieved through the use of oxygenated fuels and enhanced fuel/charge-gas mixing upstream of the lift-off length. Enhanced mixing can be obtained via higher injection pressures, smaller injector orifice diameters, lower intake-manifold and coolant temperatures, and/ormore » more retarded injection timings. This study focuses on the effects of an oxygenated fuel blend (T50) made up of 50% by volume tri-propylene glycol mono-methyl ether with a #2 ULSD emissions-certification fuel (CFA), compared against baseline testing of the CFA fuel without the oxygenate. Experimental measurements include crank-angle resolved natural luminosity (NL) and chemiluminescence (CL) imaging diagnostics. EGR is simulated by adding nitrogen and carbon dioxide to the intake charge to produce a 16% intake-oxygen mole fraction (XO2), and results are compared against cases with no charge dilution (i.e., 21% XO2). Initial experiments with a two-hole tip achieved soot-free LLFC at low loads with the T50 fuel, 240 MPa injection pressure, 50 °C intake-manifold temperature (IMT), 95 °C coolant temperature, and -5 crank-angle degree (CAD) after top-dead-center (ATDC) start of combustion (SOC) timing. The strategy was extended to more moderate loads by employing a 6-hole injector tip, where lowering the IMT to 30 °C, reducing the coolant temperature to 85 °C, and retarding the SOC timing to +5 CAD ATDC resulted in sustained LLFC at both 21% and 16% XO2 at up to 6.2 bar gross indicated mean effective pressure (gIMEP) with T50. The achievement of LLFC was confirmed by independent soot measurements using a smoke meter, spatially integrated natural luminosity from the NL diagnostics, and laser-induced incandescence for measuring soot volume fraction in the exhaust stream. In contrast to the results with T50, LLFC was not achieved under any of the test conditions with CFA. Combustion was stable under LLFC conditions, with a coefficient of variation of gIMEP less than 1.5%. Nitrogen oxides and hydrocarbon emissions were also lowered by up to 25% each for LLFC with T50 relative to using the same operating conditions with CFA. Combustion noise was similarly reduced by 4-6 dBA, and ringing intensity by 60-80%, for LLFC with T50.« less

Polycyclic aromatic hydrocarbon and particulate emissions from two-stage combustion of polystyrene: the effect of the primary furnace temperature.

PubMed

Wang, J; Levendis, Y A; Richter, H; Howard, J B; Carlson, J

2001-09-01

A study is presented on laboratory-scale combustion of polystyrene (PS) to identify staged-combustion conditions that minimize emissions. Batch combustion of shredded PS was conducted in fixed beds placed in a bench-scale electrically heated horizontal muffle furnace. In most cases, combustion of the samples occurred by forming gaseous diffusion flames in atmospheric pressure air. The combustion effluent was mixed with additional air, and it was channeled to a second muffle furnace (afterburner) placed in series. Further reactions took place in the secondary furnace at a residence time of 0.7 s. The gas temperature of the primary furnace was varied in the range of 500-1,000 degrees C, while that of the secondary furnace was kept fixed at 1,000 degrees C. Sampling for CO, CO2, O2, soot, and unburned hydrocarbon emissions (volatile and semivolatile, by GC-MS) was performed at the exits of the two furnaces. Results showed that the temperature of the primary furnace, where PS gasifies, is of paramount importance to the formation and subsequent emissions of organic species and soot. Atthe lowesttemperatures explored, mostly styrene oligomers were identified at the outlet of the primary furnace, but they did not survive the treatment in the secondary furnace. The formation and emission of polycyclic aromatic hydrocarbons (PAH) and soot were suppressed. As the temperature in the first furnace was raised, increasing amounts of a wide range of both unsubstituted and substituted PAH containing up to at least seven condensed aromatic rings were detected. A similar trend was observed for total particulate yields. The secondary furnace treatment reduced the yields of total PAH, but it had an ambiguous effect on individual species. While most low molecular mass PAH were reduced in the secondary furnace, concentrations of some larger PAH increased under certain conditions. Thus, care in the selection of operating conditions of both the primary furnace (gasifier/ burner) and the secondary furnace (afterburner) must be exercised to minimize the emission of hazardous pollutants. The emissions of soot were also reduced in the afterburner but not drastically. This indicates that soot is indeed resistant to oxidation; thus, it would be best to avoid its formation in the first place. An oxidative pyrolysis temperature of PS in the vicinity of 600 degrees C appears to accomplish exactly that. An additional afterburner treatment at a sufficiently high temperature (1,000 degrees C) may be a suitable setting for minimization of most pollutants. To obtain deeper understanding of chemical processes, the experimental results were qualitatively compared with preliminary predictions of a detailed kinetic model that describes formation and destruction pathways of chemical species including most PAH observed in the present work. The modeling was performed forthe secondary furnace assuming plug-flow conditions therein. The experimentally determined chemical composition at the outlet of the primary furnace was part of the input parameters of the model calculation.

Leaner Lifted-Flame Combustion Enabled by the Use of an Oxygenated Fuel in an Optical CI Engine

DOE PAGES

Gehmlich, Ryan K.; Dumitrescu, Cosmin E.; Wang, Yefu; ...

2016-04-05

Leaner lifted-flame combustion (LLFC) is a mixing-controlled combustion strategy for compression-ignition engines that does not produce soot because the equivalence ratio at the lift-off length, Φ(H), is less than or equal to approximately two. In addition to preventing soot formation, LLFC can simultaneously control emissions of nitrogen oxides because it is tolerant to the use of exhaust-gas recirculation for lowering in-cylinder temperatures. LLFC can be achieved through the use of oxygenated fuels and enhanced fuel/charge-gas mixing upstream of the lift-off length. Enhanced mixing can be obtained via higher injection pressures, smaller injector orifice diameters, lower intake-manifold and coolant temperatures, and/ormore » more retarded injection timings. This study focuses on the effects of an oxygenated fuel blend (T50) made up of 50% by volume tri-propylene glycol mono-methyl ether with a #2 ULSD emissions-certification fuel (CFA), compared against baseline testing of the CFA fuel without the oxygenate. Experimental measurements include crank-angle resolved natural luminosity (NL) and chemiluminescence (CL) imaging diagnostics. EGR is simulated by adding nitrogen and carbon dioxide to the intake charge to produce a 16% intake-oxygen mole fraction (XO2), and results are compared against cases with no charge dilution (i.e., 21% XO2). Initial experiments with a two-hole tip achieved soot-free LLFC at low loads with the T50 fuel, 240 MPa injection pressure, 50 °C intake-manifold temperature (IMT), 95 °C coolant temperature, and -5 crank-angle degree (CAD) after top-dead-center (ATDC) start of combustion (SOC) timing. The strategy was extended to more moderate loads by employing a 6-hole injector tip, where lowering the IMT to 30 °C, reducing the coolant temperature to 85 °C, and retarding the SOC timing to +5 CAD ATDC resulted in sustained LLFC at both 21% and 16% XO2 at up to 6.2 bar gross indicated mean effective pressure (gIMEP) with T50. The achievement of LLFC was confirmed by independent soot measurements using a smoke meter, spatially integrated natural luminosity from the NL diagnostics, and laser-induced incandescence for measuring soot volume fraction in the exhaust stream. In contrast to the results with T50, LLFC was not achieved under any of the test conditions with CFA. Combustion was stable under LLFC conditions, with a coefficient of variation of gIMEP less than 1.5%. Nitrogen oxides and hydrocarbon emissions were also lowered by up to 25% each for LLFC with T50 relative to using the same operating conditions with CFA. Combustion noise was similarly reduced by 4-6 dBA, and ringing intensity by 60-80%, for LLFC with T50.« less

The solid surface combustion experiment aboard the USML-1 mission

NASA Technical Reports Server (NTRS)

Altenkirch, Robert A.; Sacksteder, Kurt; Bhattacharjee, Subrata; Ramachandra, Prashant A.; Tang, Lin; Wolverton, M. Katherine

1994-01-01

AA Experimental results from the five experiments indicate that flame spread rate increases with increasing ambient oxygen content and pressure. An experiment was conducted aboard STS-50/USML-1 in the solid Surface Combustion Experiment (SSCE) hardware for flame spread over a thin cellulosic fuel in a quiescent oxidizer of 35% oxygen/65% nitrogen at 1.0 atm. pressure in microgravity. The USML-1 test was the fourth of five planned experiments for thin fuels, one performed during each of five Space Shuttle Orbiter flights. Data that were gathered include gas- and solid-phase temperatures and motion picture flame images. Observations of the flame are described and compared to theoretical predictions from steady and unsteady models that include flame radiation from CO2 and H2O. Experimental results from the five esperiments indicate that flame spread rate increases with increasing ambient oxygen content and pressure. The brightness of the flame and the visible soot radiation also increase with increasing spread rate. Steady-state numerical predictions of temperature and spread rate and flame structure trends compare well with experimental results near the flame's leading edge while gradual flame evolution is captured through the unsteady model.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaplan, C.R.; Shaddix, C.R.; Smyth, K.C.

This paper presents time-dependent numerical simulations of both steady and time-varying CH{sub 4}/air diffusion flames to examine the differences in combustion conditions which lead to the observed enhancement in soot production in the flickering flames. The numerical model solves the two-dimensional, time-dependent, reactive-flow Navier-Stokes equations coupled with submodels for soot formation and radiation transport. Qualitative comparisons between the experimental and computed steady flame show good agreement for the soot burnout height and overall flame shape except near the burner lip. Quantitative comparisons between experimental and computed radial profiles of temperature and soot volume fraction for the steady flame show goodmore » to excellent agreement at mid-flame heights, but some discrepancies near the burner lip and at high flame heights. For the time-varying CH{sub 4}/air flame, the simulations successfully predict that the maximum soot concentration increases by over four times compared to the steady flame with the same mean fuel and air velocities. By numerically tracking fluid parcels in the flowfield, the temperature and stoichiometry history were followed along their convective pathlines. Results for the pathline which passes through the maximum sooting region show that flickering flames exhibit much longer residence times during which the local temperatures and stoichiometries are favorable for soot production. The simulations also suggest that soot inception occurs later in flickering flames, and at slightly higher temperatures and under somewhat leaner conditions compared to the steady flame. The integrated soot model of Syed et al., which was developed from a steady CH{sub 4}/air flame, successfully predicts soot production in the time-varying CH{sub 4}/air flames.« less

Soot Volume Fraction Maps for Normal and Reduced Gravity Laminar Acetylene Jet Diffusion Flames

NASA Technical Reports Server (NTRS)

Greenberg, Paul S.; Ku, Jerry C.

1997-01-01

The study of soot particulate distribution inside gas jet diffusion flames is important to the understanding of fundamental soot particle and thermal radiative transport processes, as well as providing findings relevant to spacecraft fire safety, soot emissions, and radiant heat loads for combustors used in air-breathing propulsion systems. Compared to those under normal gravity (1-g) conditions, the elimination of buoyancy-induced flows is expected to significantly change the flow field in microgravity (O g) flames, resulting in taller and wider flames with longer particle residence times. Work by Bahadori and Edelman demonstrate many previously unreported qualitative and semi-quantitative results, including flame shape and radiation, for sooting laminar zas jet diffusion flames. Work by Ku et al. report soot aggregate size and morphology analyses and data and model predictions of soot volume fraction maps for various gas jet diffusion flames. In this study, we present the first 1-g and 0-g comparisons of soot volume fraction maps for laminar acetylene and nitrogen-diluted acetylene jet diffusion flames. Volume fraction is one of the most useful properties in the study of sooting diffusion flames. The amount of radiation heat transfer depends directly on the volume fraction and this parameter can be measured from line-of-sight extinction measurements. Although most Soot aggregates are submicron in size, the primary particles (20 to 50 nm in diameter) are in the Rayleigh limit, so the extinction absorption) cross section of aggregates can be accurately approximated by the Rayleigh solution as a function of incident wavelength, particles' complex refractive index, and particles' volume fraction.

Climatic Effects of Medium-Sized Asteroid Impacts on Land

NASA Astrophysics Data System (ADS)

Bardeen, C.; Garcia, R. R.; Toon, O. B.; Otto-Bliesner, B. L.; Wolf, E. T.

2015-12-01

Using the Community Earth System Model (CESM), a three-dimensional coupled climate model with interactive chemistry, we have simulated the climate response to a medium-sized (1 km) asteroid impact on the land. An impact of this size would cause local fires and may also generate submicron dust particles. Dust aerosols are injected into the upper atmosphere where they persist for ~3 years. Soot aerosols from fires are injected into the troposphere and absorb solar radiation heating the air which helps loft the soot into the stratosphere where it persists for ~10 years. Initially, these aerosols cause a heating of over 240 K in the stratosphere and up to a 70% reduction in downwelling solar radiation at the surface. Global average surface temperature cools by as much as -8.5 K, ocean temperature cools by -4.5 K, precipitation is reduced by 50%, and the ozone column is reduced by 55%. The surface UV Index exceeds 20 in the tropics for several years. These changes represent a significant hazard to life on a global scale. These results extend the work of Pierazzo et al. (2010), also using CESM, which found a significant impact on stratospheric ozone, but little change in surface temperature or precipitation, from a 1 km asteroid impact in the ocean.

Changes of ns-soot mixing states and shapes in an urban area during CalNex

NASA Astrophysics Data System (ADS)

Adachi, Kouji; Buseck, Peter R.

2013-05-01

Aerosol particles from megacities influence the regional and global climate as well as the health of their occupants. We used transmission electron microscopes (TEMs) to study aerosol particles collected from the Los Angeles area during the 2010 CalNex campaign. We detected major amounts of ns-soot, defined as consisting of carbon nanospheres, sulfate, sea salt, and organic aerosol (OA) and lesser amounts of brochosome particles from leaf hoppers. Ns-soot-particle shapes, mixing states, and abundances varied significantly with sampling times and days. Within plumes having high CO2 concentrations, much ns-soot was compacted and contained a relatively large number of carbon nanospheres. Ns-soot particles from both CalNex samples and Mexico City, the latter collected in 2006, had a wide range of shapes when mixed with other aerosol particles, but neither sets showed spherical ns-soot nor the core-shell configuration that is commonly used in optical calculations. Our TEM observations and light-absorption calculations of modeled particles indicate that, in contrast to ns-soot particles that are embedded within other materials or have the hypothesized core-shell configurations, those attached to other aerosol particles hardly enhance their light absorption. We conclude that the ways in which ns-soot mixes with other particles explain the observations of smaller light amplification by ns-soot coatings than model calculations during the CalNex campaign and presumably in other areas.

Refractive indices at visible wavelengths of soot emitted from buoyant turbulent diffusion flames

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, J.S.; Krishnan, S.K.; Faeth, G.M.

1996-11-01

Measurements of the optical properties of soot, emphasizing refractive indices, are reported for visible wavelengths. The experiments considered soot in the fuel-lean (overfire) region of buoyant turbulent diffusion flames in the long residence time regime where soot properties are independent of position in the overfire region and residence time. Flames fueled with acetylene, propylene, ethylene and propane burning in still air provided a range of soot physical and structure properties. Measurements included soot composition, density, structure, gravimetric volume fraction, scattering properties and absorption properties. These data were analyzed to find soot fractal dimensions, refractive indices and dimensionless extinction coefficients, assumingmore » Rayleigh-Debye-Gans scattering for polydisperse mass fractal aggregates (RDG-PFA theory). RDG-PFA theory was successfully evaluated, based on measured scattering patterns. Soot fractal dimensions were independent of both fuel type and wavelength, yielding a mean value of 1.77 with a standard deviation of 0.04. Refractive indices were independent of fuel type within experimental uncertainties and were in reasonably good agreement with earlier measurements for soot in the fuel-lean region of diffusion flames due to Dalzell and Sarofim (1969). Dimensionless extinction coefficients were independent of both fuel type and wavelength, yielding a mean value of 5.1 with a standard deviation of 0.5, which is lower than earlier measurements for reasons that still must be explained.« less

Laminar Soot Processes Experiment Shedding Light on Flame Radiation

NASA Technical Reports Server (NTRS)

Urban, David L.

1998-01-01

The Laminar Soot Processes (LSP) experiment investigated soot processes in nonturbulent, round gas jet diffusion flames in still air. The soot processes within these flames are relevant to practical combustion in aircraft propulsion systems, diesel engines, and furnaces. However, for the LSP experiment, the flames were slowed and spread out to allow measurements that are not tractable for practical, Earth-bound flames.

Effect of Sulfuric Acid on the Uptake of Sulfur Dioxide on Soot

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Koehler, B. G.

2001-05-01

The uptake of SO2 on soot may lead to the formation of sulfuric acid on the soot. The sulfuric acid then can affect the further uptake of SO2 on the soot. We are interested in the effect of submonolayer H2SO4 on the uptake of SO2. We measured the uptake of SO2 on n-hexane soot as a function SO2 pressure (10-7 to 10-4 Torr) and sulfuric acid coverage between -140\\deg and -120\\deg C. We generate sulfuric acid by adsorbing varying amounts of SO3 on soot, covering the SO3 with a thick layer of condensed H2O, and heating to 193 K to react the SO3 and H2O and to remove the excess H2O. The sulfuric acid coverage is in the range of monolayer or sub-monolayer. Adsorption of SO2 on soot with and without the sulfuric acid shows that the acid reduces the SO2 uptake by a factor of two or more. Varying the amount of acid has little effect on uptake. However, increasing the thickness of the soot substrate causes a significant increase in SO2 uptake.

Laser-induced incandescence measurements of soot in turbulent pool fires.

PubMed

Frederickson, Kraig; Kearney, Sean P; Grasser, Thomas W

2011-02-01

We present what we believe to be the first application of the laser-induced incandescence (LII) technique to large-scale fire testing. The construction of an LII instrument for fire measurements is presented in detail. Soot volume fraction imaging from 2 m diameter pool fires burning blended toluene/methanol liquid fuels is demonstrated along with a detailed report of measurement uncertainty in the challenging pool fire environment. Our LII instrument relies upon remotely located laser, optical, and detection systems and the insertion of water-cooled, fiber-bundle-coupled collection optics into the fire plume. Calibration of the instrument was performed using an ethylene/air laminar diffusion flame produced by a Santoro-type burner, which allowed for the extraction of absolute soot volume fractions from the LII images. Single-laser-shot two-dimensional images of the soot layer structure are presented with very high volumetric spatial resolution of the order of 10(-5) cm3. Probability density functions of the soot volume fraction fluctuations are constructed from the large LII image ensembles. The results illustrate a highly intermittent soot fluctuation field with potentially large macroscale soot structures and clipped soot probability densities.

Prediction of soot and thermal radiation in a model gas turbine combustor burning kerosene fuel spray at different swirl levels

NASA Astrophysics Data System (ADS)

Ghose, Prakash; Patra, Jitendra; Datta, Amitava; Mukhopadhyay, Achintya

2016-05-01

Combustion of kerosene fuel spray has been numerically simulated in a laboratory scale combustor geometry to predict soot and the effects of thermal radiation at different swirl levels of primary air flow. The two-phase motion in the combustor is simulated using an Eulerian-Lagragian formulation considering the stochastic separated flow model. The Favre-averaged governing equations are solved for the gas phase with the turbulent quantities simulated by realisable k-ɛ model. The injection of the fuel is considered through a pressure swirl atomiser and the combustion is simulated by a laminar flamelet model with detailed kinetics of kerosene combustion. Soot formation in the flame is predicted using an empirical model with the model parameters adjusted for kerosene fuel. Contributions of gas phase and soot towards thermal radiation have been considered to predict the incident heat flux on the combustor wall and fuel injector. Swirl in the primary flow significantly influences the flow and flame structures in the combustor. The stronger recirculation at high swirl draws more air into the flame region, reduces the flame length and peak flame temperature and also brings the soot laden zone closer to the inlet plane. As a result, the radiative heat flux on the peripheral wall decreases at high swirl and also shifts closer to the inlet plane. However, increased swirl increases the combustor wall temperature due to radial spreading of the flame. The high incident radiative heat flux and the high surface temperature make the fuel injector a critical item in the combustor. The injector peak temperature increases with the increase in swirl flow mainly because the flame is located closer to the inlet plane. On the other hand, a more uniform temperature distribution in the exhaust gas can be attained at the combustor exit at high swirl condition.

Chromatic variation of soot soiling: a possible marker for gunshot wounds in burnt bone.

PubMed

Amadasi, Alberto; Merli, Daniele; Brandone, Alberto; Cattaneo, Cristina

2014-01-01

Soot soiling is a crucial forensic parameter around gunshot lesions. Carbonization, however, can severely alter human tissues and mimic such clues. This study aims at evaluating the survival of soot soiling even after carbonization in bone. A total of 36 bovine ribs (half fleshed and half defleshed) were shot with two types of bullet (both 9-mm; full metal-jacketed and unjacketed) with a near-contact range. With unjacketed bullets, the shot left in every case a clear, black, and roughly round soot stain around the entrance wound, whereas full metal-jacketed bullets left no signs of soot. Every specimen then underwent calcination in an oven at 800°C. The analysis of the charred samples clearly showed the survival of the soot soiling in both fleshed and bony samples, with a clear correspondence with the former position, but with a different color (yellow). Thus, soot soiling may survive, although with a different color, even after charring. © 2013 American Academy of Forensic Sciences.

Effects of morphology and wavelength on the measurement accuracy of soot volume fraction by laser extinction

NASA Astrophysics Data System (ADS)

Wang, Ya-fei; Huang, Qun-xing; Wang, Fei; Chi, Yong; Yan, Jian-hua

2018-01-01

A novel method to evaluate the quantitative effects of soot morphology and incident wavelength on the measurement accuracy of soot volume fraction, by the laser extinction (LE) technique is proposed in this paper. The results indicate that the traditional LE technique would overestimate soot volume fraction if the effects of morphology and wavelength are not considered. Before the agglomeration of isolated soot primary particles, the overestimation of the LE technique is in the range of 2-20%, and rises with increasing primary particle diameter and with decreasing incident wavelength. When isolated primary particles are agglomerated into fractal soot aggregates, the overestimation would exceed 30%, and rise with increasing primary particle number per soot aggregate, fractal dimension and fractal prefactor and with decreasing incident wavelength to a maximum value of 55%. Finally, based on these results above, the existing formula of the LE technique gets modified, and the modification factor is 0.65-0.77.

Laboratory measurements in a turbulent, swirling flow. [measurement of soot inside a flame-tube burner

NASA Technical Reports Server (NTRS)

Hoult, D. P.

1979-01-01

Measurements of soot inside a flame-tube burner using a special water-flushed probe are discussed. The soot is measured at a series of points at each burner, and upon occasion gaseous constitutents NO, CO, hydrocarbons, etc., were also measured. Four geometries of flame-tube burners were studied, as well as a variety of different fuels. The role of upstream geometry on the downstream pollutant formation was studied. It was found that the amount of soot formed in particularly sensitive to how aerodynamically clean the configuration of the burner is upstream of the injector swirl vanes. The effect of pressure on soot formation was also studied. It was found that beyond a certain Reynolds number, the peak amount of soot formed in the burner is constant.

Effects of Fuel Preheat on Soot Formation in Microgravity Laminar Diffusion Flames

NASA Technical Reports Server (NTRS)

Konsur, Bogdan; Megaridis, Constantine M.; Griffin, DeVon W.

1997-01-01

Nonbuoyant flames offer themselves as an attractive and promising platform to gain a better understanding of soot mechanisms. The effects of buoyancy can be eliminated temporarily in drop towers which sustain brief intervals of reduced gravity-typically lower than 10(exp -3)g- extending up to several seconds at a time. Microgravity facilities have been employed to show that nonbuoyant flames are longer, wider and sootier than their normal-gravity counterparts. Sunderland et al. recently verified the existence of smoke point in laminar nonbuoyant flames. As reported, microgravity flames operating above their smoke point displayed a blunt tip and much broader soot-containing regimes in comparison to their buoyant counterparts. Mortazavi et al. established that residence times in microgravity laminar jet diffusion flames with Re=0(100) tend to be proportional to burner diameter and inversely proportional to burner exit velocity. This offers the capability to alter residence times in nonbuoyant laminar jet diffusion flames when varying the burner exit diameters and velocities. Megaridis et al. presented a quantitative definition of the soot-field structure within laminar microgravity jet diffusion flames which operated well above their smoke point. The experimental methodology involved a full-field laser-light extinction technique and jet diffusion flames of nitrogen-diluted (50% vol.) acetylene fuel burning in quiescent air at atmospheric pressure. The work was conducted at the 2.2s drop tower of the NASA Lewis Research Center (NASA-LeRC). Parallel work on 1-g flames was also presented in (6) to facilitate comparisons on the effect of gravity on the soot fields. As reported, the soot spatial distributions in 0-g flames did not change in a detectable manner after 1s within a typical 2.2s experiment. During that period, the soot field was shown to sustain a pronounced annular structure throughout the luminous nonbuoyant-flame zone. The maximum soot volume fraction measured at 0-g was nearly a factor of two higher than that at 1-g, thus confirming the enhanced sooting tendency of nonbuoyant flames. Greenberg and Ku presented a similar study and reported trends that matched those of for the 50% (vol.) nitrogen-diluted acetylene fuel. Furthermore, they examined pure acetylene flames and reported similar trends with respect to the influence of gravity on maximum soot volume fractions and flame cross-section-averaged soot loadings. Both studies clearly demonstrated the improved spatial resolution of microgravity flames compared to their normal-gravity counterparts. The current study evaluates the influence of moderate fuel preheat on soot formation within 0-g laminar gas jet diffusion flames. While fuel temperature variations have little influence on residence times in 1-g, they have a much more significant effect in 0-g. The primary objective of this program is to quantify this effect and its consequences on sooting by comparing soot volume fraction distributions under preheated and unpreheated-fuel conditions. Furthermore, the current work aims at expanding the limited soot database available for nonbuoyant flames. Soot fields in such flames can be used to perform additional tests of recently developed soot sub-models which have the potential to become powerful predicting tools in combustion design.

A quantitative estimation of the exhaust, abrasion and resuspension components of particulate traffic emissions using electron microscopy

NASA Astrophysics Data System (ADS)

Weinbruch, Stephan; Worringen, Annette; Ebert, Martin; Scheuvens, Dirk; Kandler, Konrad; Pfeffer, Ulrich; Bruckmann, Peter

2014-12-01

The contribution of the three traffic-related components exhaust, abrasion, and resuspension to kerbside and urban background PM10 and PM1 levels was quantified based on the analysis of individual particles by scanning electron microscopy. A total of 160 samples was collected on 38 days between February and September 2009 at a kerbside and an urban background station in the urban/industrial Ruhr area (Germany). Based on size, morphology, chemical composition and stability under electron bombardment, the 111,003 particles studied in detail were classified into the following 14 particle classes: traffic/exhaust, traffic/abrasion, traffic/resuspension, carbonaceous/organic, industry/metallurgy, industry/power plants, secondary particles, (aged) sea salt, silicates, Ca sulfates, carbonates, Fe oxides/hydroxides, biological particles, and other particles. The traffic/exhaust component consists predominantly of externally mixed soot particles and soot internally mixed with secondary particles. The traffic/abrasion component contains all particles with characteristic tracer elements (Fe, Cu, Ba, Sb, Zn) for brake and tire abrasion. The traffic/resuspension component is defined by the mixing state and comprises all internally mixed particles with a high proportion of silicates or Fe oxides/hydroxides which contain soot or abrasion particles as minor constituent. In addition, silicates and Fe oxides/hydroxides internally mixed with chlorine and sulphur containing particles were also assigned to the traffic/resuspension component. The total contribution of traffic to PM10 was found to be 27% at the urban background station and 48% at the kerbside station, the corresponding values for PM1 are 15% and 39%. These values lie within the range reported in previous literature. The relative share of the different traffic components for PM10 at the kerbside station was 27% exhaust, 15% abrasion, and 58% resuspension (38%, 8%, 54% for PM1). For the urban background, the following relative shares were obtained for PM10: 22% exhaust, 22% abrasion and 56% resuspension (40%, 27%, 33% for PM1). Compared to previous publications we have observed a significantly lower portion of exhaust particles and a significantly higher portion of resuspension particles. The high abundance of resuspension particles underlines their significance for the observed adverse health effects of traffic emissions and for mitigation measures.

LES of Sooting Flames

DTIC Science & Technology

2006-12-01

27], [28] on soot nucleation, and [29] on the soot formation in diesel engines . [27] discussed the unresolved problems in SOx, NOx , and soot...used LEM approach to study aerosol dynamics in engine exhaust plumes. Recently, [41] used detailed NOx mechanism combined with MOM to predict the...combustion engines . For instance, the laminar flamelet approach used by [43, 44, 45], allows the usage of a detailed chemical mechanism but is not

Hydrodynamic Suppression of Soot Formation in Laminar Coflowing Jet Diffusion Flames. Appendix C

NASA Technical Reports Server (NTRS)

Dai, Z.; Faeth, G. M.; Yuan, Z.-G. (Technical Monitor); Urban, D. L. (Technical Monitor); Yuan, Z.-G. (Technical Monitor)

2000-01-01

Effects of flow (hydrodynamic) properties on limiting conditions for soot-free laminar non-premixed hydrocarbon/air flames (called laminar soot-point conditions) were studied, emphasizing non-buoyant laminar coflowing jet diffusion flames. Effects of air/fuel-stream velocity ratios were of particular interest; therefore, the experiments were carried out at reduced pressures to minimize effects of flow acceleration due to the intrusion of buoyancy. Test conditions included reactant temperatures of 300 K; ambient pressures of 3.7-49 8 kPa; methane-, acetylene-, ethylene-, propane-, and methane-fueled flames burning in coflowing air with fuel-port diameters of 1.7, 3.2, and 6.4 mm, fuel jet Reynolds numbers of 18-121; air coflow velocities of 0-6 m/s; and air/fuel-stream velocity ratios of 0.003-70. Measurements included laminar soot-point flame lengths, laminar soot-point fuel flow rates, and laminar liftoff conditions. The measurements show that laminar soot-point flame lengths and fuel flow rates can be increased, broadening the range of fuel flow rates where the flames remain soot free, by increasing air/fuel-stream velocity ratios. The mechanism of this effect involves the magnitude and direction of flow velocities relative to the flame sheet where increased air/fuel-stream velocity ratios cause progressive reduction of flame residence times in the fuel-rich soot-formation region. The range of soot-free conditions is limited by both liftoff, particularly at low pressures, and the intrusion of effects of buoyancy on effective air/fuel-stream velocity ratios, particularly at high pressures. Effective correlations of laminar soot- and smoke-point flame lengths were also found in terms of a corrected fuel flow rate parameter, based on simplified analysis of laminar jet diffusion flame structure. The results show that laminar smoke-point flame lengths in coflowing air environments are roughly twice as long as soot-free (blue) flames under comparable conditions due to the presence of luminous soot particles under fuel-lean conditions when smoke-point conditions are approached. This is very similar to earlier findings concerning differences between laminar smoke- and sootpoint flame lengths in still environments.

Gas and Particulate Aircraft Emissions Measurements: Impacts on local air quality.

NASA Astrophysics Data System (ADS)

Jayne, J. T.; Onasch, T.; Northway, M.; Canagaratna, M.; Worsnop, D.; Timko, M.; Wood, E.; Miake-Lye, R.; Herndon, S.; Knighton, B.; Whitefield, P.; Hagen, D.; Lobo, P.; Anderson, B.

2007-12-01

Air travel and freight shipping by air are becoming increasingly important and are expected to continue to expand. The resulting increases in the local concentrations of pollutants, including particulate matter (PM), volatile organic compounds (VOCs), and nitrogen oxides (NOX), can have negative impacts on regional air quality, human health and can impact climate change. In order to construct valid emission inventories, accurate measurements of aircraft emissions are needed. These measurements must be done both at the engine exit plane (certification) and downwind following the rapid cooling, dilution and initial atmospheric processing of the exhaust plume. We present here results from multiple field experiments which include the Experiment to Characterize Volatile Aerosol and Trace Species Emissions (EXCAVATE) and the four Aircraft Particle Emissions eXperiments (APEX- 1/Atlanta/2/3) which characterized gas and particle emissions from both stationary or in-use aircraft. Emission indices (EIs) for NOx and VOCs and for particle number concentration, refractory PM (black carbon soot) and volatile PM (primarily sulfate and organic) particles are reported. Measurements were made at the engine exit plane and at several downstream locations (10 and 30 meters) for a number of different engine types and engine thrust settings. A significant fraction of organic particle mass is composed of low volatility oil-related compounds and is not combustion related, potentially emitted by vents or heated surfaces within aircraft engines. Advected plumes measurements from in-use aircraft show that the practice of reduced thrust take-offs has a significant effect on total NOx and soot emitted in the vicinity of the airport. The measurements reported here represent a first observation of this effect and new insights have been gained with respect to the chemical processing of gases and particulates important to the urban airshed.

Perovskite-type catalytic materials for environmental applications.

PubMed

Labhasetwar, Nitin; Saravanan, Govindachetty; Kumar Megarajan, Suresh; Manwar, Nilesh; Khobragade, Rohini; Doggali, Pradeep; Grasset, Fabien

2015-06-01

Perovskites are mixed-metal oxides that are attracting much scientific and application interest owing to their low price, adaptability, and thermal stability, which often depend on bulk and surface characteristics. These materials have been extensively explored for their catalytic, electrical, magnetic, and optical properties. They are promising candidates for the photocatalytic splitting of water and have also been extensively studied for environmental catalysis applications. Oxygen and cation non-stoichiometry can be tailored in a large number of perovskite compositions to achieve the desired catalytic activity, including multifunctional catalytic properties. Despite the extensive uses, the commercial success for this class of perovskite-based catalytic materials has not been achieved for vehicle exhaust emission control or for many other environmental applications. With recent advances in synthesis techniques, including the preparation of supported perovskites, and increasing understanding of promoted substitute perovskite-type materials, there is a growing interest in applied studies of perovskite-type catalytic materials. We have studied a number of perovskites based on Co, Mn, Ru, and Fe and their substituted compositions for their catalytic activity in terms of diesel soot oxidation, three-way catalysis, N 2 O decomposition, low-temperature CO oxidation, oxidation of volatile organic compounds, etc. The enhanced catalytic activity of these materials is attributed mainly to their altered redox properties, the promotional effect of co-ions, and the increased exposure of catalytically active transition metals in certain preparations. The recent lowering of sulfur content in fuel and concerns over the cost and availability of precious metals are responsible for renewed interest in perovskite-type catalysts for environmental applications.

Perovskite-type catalytic materials for environmental applications

PubMed Central

Labhasetwar, Nitin; Saravanan, Govindachetty; Kumar Megarajan, Suresh; Manwar, Nilesh; Khobragade, Rohini; Doggali, Pradeep; Grasset, Fabien

2015-01-01

Perovskites are mixed-metal oxides that are attracting much scientific and application interest owing to their low price, adaptability, and thermal stability, which often depend on bulk and surface characteristics. These materials have been extensively explored for their catalytic, electrical, magnetic, and optical properties. They are promising candidates for the photocatalytic splitting of water and have also been extensively studied for environmental catalysis applications. Oxygen and cation non-stoichiometry can be tailored in a large number of perovskite compositions to achieve the desired catalytic activity, including multifunctional catalytic properties. Despite the extensive uses, the commercial success for this class of perovskite-based catalytic materials has not been achieved for vehicle exhaust emission control or for many other environmental applications. With recent advances in synthesis techniques, including the preparation of supported perovskites, and increasing understanding of promoted substitute perovskite-type materials, there is a growing interest in applied studies of perovskite-type catalytic materials. We have studied a number of perovskites based on Co, Mn, Ru, and Fe and their substituted compositions for their catalytic activity in terms of diesel soot oxidation, three-way catalysis, N2O decomposition, low-temperature CO oxidation, oxidation of volatile organic compounds, etc. The enhanced catalytic activity of these materials is attributed mainly to their altered redox properties, the promotional effect of co-ions, and the increased exposure of catalytically active transition metals in certain preparations. The recent lowering of sulfur content in fuel and concerns over the cost and availability of precious metals are responsible for renewed interest in perovskite-type catalysts for environmental applications. PMID:27877813

Shapes of Nonbuoyant Round Luminous Hydrocarbon/Air Laminar Jet Diffusion Flames

NASA Technical Reports Server (NTRS)

Lin, K.-C.; Faeth, G. M.; Sunderland, P. B.; Urban, D. L.; Yuan, Z.-G.

1999-01-01

The shapes (luminous flame boundaries) of round luminous nonbuoyant soot-containing hydrocarbon/air laminar jet diffusion flames at microgravity were found from color video images obtained on orbit in the Space Shuttle Columbia. Test conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K, ambient pressures of 35-130 kPa, initial jet diameters of 1.6 and 2.7 mm, and jet exit Reynolds numbers of 45-170. Present test times were 100-200 s and yielded steady axisymmetric flames that were close to the laminar smoke point (including flames both emitting and not emitting soot) with luminous flame lengths of 15-63 mm. The present soot-containing flames had larger luminous flame lengths than earlier ground-based observations having similar burner configurations: 40% larger than the luminous flame lengths of soot-containing low gravity flames observed using an aircraft (KC-135) facility due to reduced effects of accelerative disturbances and unsteadiness; roughly twice as large as the luminous flame lengths of soot-containing normal gravity flames due to the absence of effects of buoyant mixing and roughly twice as large as the luminous flame lengths of soot-free low gravity flames observed using drop tower facilities due to the presence of soot luminosity and possible reduced effects of unsteadiness. Simplified expressions to estimate the luminous flame boundaries of round nonbuoyant laminar jet diffusion flames were obtained from the classical analysis of Spalding (1979); this approach provided Successful Correlations of flame shapes for both soot-free and soot-containing flames, except when the soot-containing flames were in the opened-tip configuration that is reached at fuel flow rates near and greater than the laminar smoke point fuel flow rate.

Shapes of Nonbuoyant Round Luminous Hydrocarbon/Air Laminar Jet Diffusion Flames. Appendix H

NASA Technical Reports Server (NTRS)

Lin, K.-C.; Faeth, G. M.; Sunderland, P. B.; Urban, D. L.; Yuan, Z.-G.; Ross, Howard B. (Technical Monitor)

2000-01-01

The shapes (luminous flame boundaries) of round luminous nonbuoyant soot-containing hydrocarbon/air laminar jet diffusion flames at microgravity were found from color video images obtained on orbit in the Space Shuttle Columbia. Test conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K ambient pressures of 35-130 kPa, initial jet diameters of 1.6 and 2.7 mm, and jet exit Reynolds numbers of 45-170. Present test times were 100-200 s and yielded steady axisymmetric flames that were close to the laminar smoke point (including flames both emitting and not emitting soot) with luminous flame lengths of 15-63 mm. The present soot-containing flames had larger luminous flame lengths than earlier ground-based observations having similar burner configurations: 40% larger than the luminous flame lengths of soot-containing low gravity flames observed using an aircraft (KC-135) facility due to reduced effects of accelerative disturbances and unsteadiness; roughly twice as large as the luminous flame lengths of soot-containing normal gravity flames due to the absence of effects of buoyant mixing and roughly twice as large as the luminous flame lengths of soot-free low gravity flames observed using drop tower facilities due to the presence of soot luminosity and possible reduced effects of unsteadiness, Simplified expressions to estimate the luminous flame boundaries of round nonbuoyant laminar jet diffusion flames were obtained from the classical analysis of Spalding; this approach provided successful correlations of flame shapes for both soot-free and soot-containing flames, except when the soot-containing flames were in the opened-tip configuration that is reached at fuel flow rates near and greater than the laminar smoke point fuel flow rate.

Soot and liquid-phase fuel distributions in a newly designed optically accessible DI diesel engine

NASA Astrophysics Data System (ADS)

Dec, J. E.; Espey, C.

1993-10-01

Two-dimensional (2-D) laser-sheet imaging has been used to examine the soot and liquid-phase fuel distributions in a newly designed, optically accessible, direct-injection diesel engine of the heavy-duty size class. The design of this engine preserves the intake port geometry and basic dimensions of a Cummins N-series production engine. It also includes several unique features to provide considerable optical access. Liquid-phase fuel and soot distribution studies were conducted at a medium speed (1,200 rpm) using a Cummins closed-nozzle fuel injector. The scattering was used to obtain planar images of the liquid-phase fuel distribution. These images show that the leading edge of the liquid-phase portion of the fuel jet reaches a maximum length of 24 mm, which is about half the combustion bowl radius for this engine. Beyond this point virtually all the fuel has vaporized. Soot distribution measurements were made at a high load condition using three imaging diagnostics: natural flame luminosity, 2-D laser-induced incandescence, and 2-D elastic scattering. This investigation showed that the soot distribution in the combusting fuel jet develops through three stages. First, just after the onset of luminous combustion, soot particles are small and nearly uniformly distributed throughout the luminous region of the fuel jet. Second, after about 2 crank angle degrees a pattern develops of a higher soot concentration of larger sized particles in the head vortex region of the jet and a lower soot concentration of smaller sized particles upstream toward the injector. Third, after fuel injection ends, both the soot concentration and soot particle size increase rapidly in the upstream portion of the fuel jet.

Multi-Wavelength Measurement of Soot Optical Properties: Influence of Non-Absorbing Coatings

NASA Astrophysics Data System (ADS)

Freedman, Andrew; Renbaum-Wollf, Lindsay; Forestieri, Sara; Lambe, Andrew; Cappa, Christopher; Davidovits, Paul; Onasch, Timothy

2015-04-01

Soot, a product of incomplete combustion, plays an important role in the earth's climate system through the absorption and scattering of solar radiation. Important in quantifying the direct radiative impacts of soot in climate models, and specifically of black carbon (BC), is the assumed BC refractive index and shape-dependent interaction of light with BC particles. The latter assumption carries significant uncertainty because BC particles are fractal-like, being agglomerates of smaller (20-40 nm) spherules, yet many optical models such as Mie theory in particular, typically assume a spherical particle morphology. It remains unclear under what conditions this is an acceptable assumption. To investigate the ability of various optical models to reproduce observed BC optical properties, we obtained measurements of light absorption, scattering and extinction coefficients and thus single scattering albedo (SSA) of size-resolved soot particles. Measurements were made on denuded soot particles produced using both methane and ethylene as fuels. In addition, these soot particles were coated with dioctyl sebacate or sulfuric acid and the enhancement in the apparent mass absorption coefficient determined. Extinction and absorption were measured using a dual cavity ringdown photoacoustic spectrometer (CRD-PAS) at 405 nm and 532 nm. Scattering and extinction were measured using a CAPS PMssa single scattering albedo monitor (Aerodyne) at 630 nm. Soot particle mass was quantified using a centrifugal particle mass analyzer (CPMA, Cambustion), mobility size with a scanning mobility particle sizer (SMPS, TSI) and soot concentration with a CPC (Brechtel). The results will be interpreted in light of both Mie theory which assumes spherical and uniform particles and Rayleigh-Debye-Gans (RDG) theory, which assumes that the absorption properties of soot are dictated by the individual spherules. For denuded soot, effective refractive indices will be determined.

Developing a predictive model for the chemical composition of soot nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Violi, Angela; Michelsen, Hope; Hansen, Nils

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 amore » 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.« less

Soot Formation in Purely-Curved Premixed Flames and Laminar Flame Speeds of Soot-Forming Flames

NASA Technical Reports Server (NTRS)

Buchanan, Thomas; Wang, Hai

2005-01-01

The research addressed here is a collaborative project between University of Delaware and Case Western Reserve University. There are two basic and related scientific objectives. First, we wish to demonstrate the suitability of spherical/cylindrical, laminar, premixed flames in the fundamental study of the chemical and physical processes of soot formation. Our reasoning is that the flame standoff distance in spherical/cylindrical flames under microgravity can be substantially larger than that in a flat burner-stabilized flame. Therefore the spherical/cylindrical flame is expected to give better spatial resolution to probe the soot inception and growth chemistry than flat flames. Second, we wish to examine the feasibility of determining the laminar flame speed of soot forming flames. Our basic assumption is that under the adiabatic condition (in the absence of conductive heat loss), the amount and dynamics of soot formed in the flame is unique for a given fuel/air mixture. The laminar flame speed can be rigorously defined as long as the radiative heat loss can be determined. This laminar flame speed characterizes the flame soot formation and dynamics in addition to the heat release rate. The research involves two integral parts: experiments of spherical and cylindrical sooting flames in microgravity (CWRU), and the computational counterpart (UD) that aims to simulate sooting laminar flames, and the sooting limits of near adiabatic flames. The computations work is described in this report, followed by a summary of the accomplishments achieved to date. Details of the microgra+ experiments will be discussed in a separate, final report prepared by the co-PI, Professor C-J. Sung of CWRU. Here only a brief discussion of these experiments will be given.

Performance and Emission Investigations of Jatropha and Karanja Biodiesels in a Single-Cylinder Compression-Ignition Engine Using Endoscopic Imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mistri, Gayatri K.; Aggarwal, Suresh K.; Longman, Douglas

Biofuels produced from non-edible sources that are cultivated on marginal lands represent a viable source of renewable and carbon-neutral energy. In this context, biodiesel obtained from Jatropha and Karanja oil seeds have received significant interest, especially in South Asian subcontinent. Both of these fuels are produced from non-edible plant seeds with high oil content, which can be grown on marginal lands. In this research, we have investigated the performance and emission characteristics of Jatropha and Karanja methyl esters (biodiesel) and their blends with diesel. Another objective is to examine the effect of long-term storage on biodiesel’s oxidative stability. The biodieselsmore » were produced at Indian Institute of Technology Kanpur, (IIT Kanpur), India, and the engine experiments were performed in a single cylinder, 4-stroke, compression ignition engine at Argonne National Laboratory (ANL), Chicago. An endoscope was used to visualize in-cylinder combustion events and examine the soot distribution. The effects of fuel and start of injection (SOI) on engine performance and emissions were investigated. Results indicated that ignition delay was shorter with biodiesel. Consequently the cylinder pressure and premixed heat release were higher for diesel compared to biodiesel. Engine performance data for biodiesel (J100, K100) and biodiesel blends (J30, K30) showed an increase in break thermal efficiency (BTE) (10.9%, 7.6% for biodiesel and blend, respectively), BSFC (13.1% and 5.6%), and NOx emission (9.8% and 12.9%), and a reduction in BSHC (8.64% and 12.9%), and BSCO (15.56% and 4.0%). The soot analysis from optical images qualitatively showed that biodiesel and blends produced less soot compared to diesel. The temperature profiles obtained from optical imaging further supported higher NOx in biodiesels and their blends compared to diesel. Additionally, the data indicated that retarding the injection timing leads to higher BSFC, but lower flame temperatures and NOx levels along with higher soot formation for all test fuels. The physicochemical properties such as fatty acid profile, cetane number, and oxygen content in biodiesels support the observed combustion and emission characteristics of the fuels tested in this study. Finally, the effect of long-term storage is found to increase the glycerol content, acid value and cetane number of the two biodiesels, indicating some oxidation of unsaturated fatty acids in the fuels.« less

Isotopic Tracing of Fuel Components in Particulate Emissions from Diesel Engines using Accelerator Mass Spectrometry (AMS)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buchholz, B A; Mueller, C J; Garbak, J.

2001-08-02

Accelerator mass spectrometry (AMS) is an isotope-ratio measurement technique developed in the late 1970s for tracing long-lived radioisotopes (e.g., {sup 14}C half life = 5760 y). The technique counts individual nuclei rather than waiting for their radioactive decay, allowing measurement of more than 100 low-level {sup 14}C samples per day (Vogel et al, 1995). The LLNL AMS system is shown in Fig.1. The contemporary quantity of {sup 14}C in living things ({sup 14}C/C = 1.2 x 10{sup -12} or 110 fmol {sup 14}C/ g C) is highly elevated compared to the quantity of {sup 14}C in petroleum-derived products. This isotopicmore » elevation is sufficient to trace the fate of bio-derived fuel components in the emissions of an engine without the use of radioactive materials. If synthesis of a fuel component from biologically-derived source material is not feasible, another approach is to purchase {sup 14}C-labeled material (e.g., dibutyl maleate (DBM)) and dilute it with petroleum-derived material to yield a contemporary level of {sup 14}C. In each case, the virtual absence of {sup 14}C in petroleum based fuels gives a very low {sup 14}C background that makes this approach to tracing fuel components practical. Regulatory pressure to significantly reduce the particulate emissions from diesel engines is driving research into understanding mechanisms of soot formation. If mechanisms are understood, then combustion modeling can be used to evaluate possible changes in fuel formulation and suggest possible fuel components that can improve combustion and reduce PM emissions. The combustion paradigm assumes that large molecules break down into small components and then build up again during soot formation. AMS allows us to label specific fuel components, including oxygenates, trace the carbon atoms, and test this combustion modeling paradigm. Volatile and non-volatile organic fractions (VOF, NVOF) in the PM can be further separated. The VOF of the PM can be oxidized with catalysts in the exhaust stream to further decrease PM. The effectiveness of exhaust stream catalysts to oxidize products from tracer fuel components can be monitored through AMS measurement of carbon in PM. The objects of this report are: (1) Determine contribution of diesel fuel components and oxygenates to soot formation; (2) Separate volatile and non-volatile fractions of soot; (3) Test combustion paradigm that all carbon and oxygen in fuel is equal; and (4) Produce data to validate combustion modeling.« less

Turbulent Radiation Effects in HSCT Combustor Rich Zone

NASA Technical Reports Server (NTRS)

Hall, Robert J.; Vranos, Alexander; Yu, Weiduo

1998-01-01

A joint UTRC-University of Connecticut theoretical program was based on describing coupled soot formation and radiation in turbulent flows using stretched flamelet theory. This effort was involved with using the model jet fuel kinetics mechanism to predict soot growth in flamelets at elevated pressure, to incorporate an efficient model for turbulent thermal radiation into a discrete transfer radiation code, and to couple die soot growth, flowfield, and radiation algorithm. The soot calculations used a recently developed opposed jet code which couples the dynamical equations of size-class dependent particle growth with complex chemistry. Several of the tasks represent technical firsts; among these are the prediction of soot from a detailed jet fuel kinetics mechanism, the inclusion of pressure effects in the soot particle growth equations, and the inclusion of the efficient turbulent radiation algorithm in a combustor code.

Simulations of sooting turbulent jet flames using a hybrid flamelet/stochastic Eulerian field method

NASA Astrophysics Data System (ADS)

Consalvi, Jean-Louis; Nmira, Fatiha; Burot, Daria

2016-03-01

The stochastic Eulerian field method is applied to simulate 12 turbulent C1-C3 hydrocarbon jet diffusion flames covering a wide range of Reynolds numbers and fuel sooting propensities. The joint scalar probability density function (PDF) is a function of the mixture fraction, enthalpy defect, scalar dissipation rate and representative soot properties. Soot production is modelled by a semi-empirical acetylene/benzene-based soot model. Spectral gas and soot radiation is modelled using a wide-band correlated-k model. Emission turbulent radiation interactions (TRIs) are taken into account by means of the PDF method, whereas absorption TRIs are modelled using the optically thin fluctuation approximation. Model predictions are found to be in reasonable agreement with experimental data in terms of flame structure, soot quantities and radiative loss. Mean soot volume fractions are predicted within a factor of two of the experiments whereas radiant fractions and peaks of wall radiative fluxes are within 20%. The study also aims to assess approximate radiative models, namely the optically thin approximation (OTA) and grey medium approximation. These approximations affect significantly the radiative loss and should be avoided if accurate predictions of the radiative flux are desired. At atmospheric pressure, the relative errors that they produced on the peaks of temperature and soot volume fraction are within both experimental and model uncertainties. However, these discrepancies are found to increase with pressure, suggesting that spectral models describing properly the self-absorption should be considered at over-atmospheric pressure.

Development and validation of a new soot formation model for gas turbine combustor simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Di Domenico, Massimiliano; Gerlinger, Peter; Aigner, Manfred

2010-02-15

In this paper a new soot formation model for gas turbine combustor simulations is presented. A sectional approach for the description of Polycyclic Aromatic Hydrocarbons (PAHs) and a two-equation model for soot particle dynamics are introduced. By including the PAH chemistry the formulation becomes more general in that the soot formation is neither directly linked to the fuel nor to C{sub 2}-like species, as it is the case in simpler soot models currently available for CFD applications. At the same time, the sectional approach for the PAHs keeps the required computational resources low if compared to models based on amore » detailed description of the PAH kinetics. These features of the new model allow an accurate yet affordable calculation of soot in complex gas turbine combustion chambers. A careful model validation will be presented for diffusion and partially premixed flames. Fuels ranging from methane to kerosene are investigated. Thus, flames with different sooting characteristics are covered. An excellent agreement with experimental data is achieved for all configurations investigated. A fundamental feature of the new model is that with a single set of constants it is able to accurately describe the soot dynamics of different fuels at different operating conditions. (author)« less

A Quantitative Model for the Prediction of Sooting Tendency from Molecular Structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

St. John, Peter C.; Kairys, Paul; Das, Dhrubajyoti D.

Particulate matter emissions negatively affect public health and global climate, yet newer fuel-efficient gasoline direct injection engines tend to produce more soot than their port-fuel injection counterparts. Fortunately, the search for sustainable biomass-based fuel blendstocks provides an opportunity to develop fuels that suppress soot formation in more efficient engine designs. However, as emissions tests are experimentally cumbersome and the search space for potential bioblendstocks is vast, new techniques are needed to estimate the sooting tendency of a diverse range of compounds. In this study, we develop a quantitative structure-activity relationship (QSAR) model of sooting tendency based on the experimental yieldmore » sooting index (YSI), which ranks molecules on a scale from n-hexane, 0, to benzene, 100. The model includes a rigorously defined applicability domain, and the predictive performance is checked using both internal and external validation. Model predictions for compounds in the external test set had a median absolute error of ~3 YSI units. An investigation of compounds that are poorly predicted by the model lends new insight into the complex mechanisms governing soot formation. Predictive models of soot formation can therefore be expected to play an increasingly important role in the screening and development of next-generation biofuels.« less

Emissions of soot particles from heat generators

NASA Astrophysics Data System (ADS)

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.

A Quantitative Model for the Prediction of Sooting Tendency from Molecular Structure

DOE PAGES

St. John, Peter C.; Kairys, Paul; Das, Dhrubajyoti D.; ...

2017-07-24

Particulate matter emissions negatively affect public health and global climate, yet newer fuel-efficient gasoline direct injection engines tend to produce more soot than their port-fuel injection counterparts. Fortunately, the search for sustainable biomass-based fuel blendstocks provides an opportunity to develop fuels that suppress soot formation in more efficient engine designs. However, as emissions tests are experimentally cumbersome and the search space for potential bioblendstocks is vast, new techniques are needed to estimate the sooting tendency of a diverse range of compounds. In this study, we develop a quantitative structure-activity relationship (QSAR) model of sooting tendency based on the experimental yieldmore » sooting index (YSI), which ranks molecules on a scale from n-hexane, 0, to benzene, 100. The model includes a rigorously defined applicability domain, and the predictive performance is checked using both internal and external validation. Model predictions for compounds in the external test set had a median absolute error of ~3 YSI units. An investigation of compounds that are poorly predicted by the model lends new insight into the complex mechanisms governing soot formation. Predictive models of soot formation can therefore be expected to play an increasingly important role in the screening and development of next-generation biofuels.« less

Morphology and mixing state of atmospheric particles: Links to optical properties and cloud processing

NASA Astrophysics Data System (ADS)

China, Swarup

Atmospheric particles are ubiquitous in Earth's atmosphere and impact the environment and the climate while affecting human health and Earth's radiation balance, and degrading visibility. Atmospheric particles directly affect our planet's radiation budget by scattering and absorbing solar radiation, and indirectly by interacting with clouds. Single particle morphology (shape, size and internal structure) and mixing state (coating by organic and inorganic material) can significantly influence the particle optical properties as well as various microphysical processes, involving cloud-particle interactions and including heterogeneous ice nucleation and water uptake. Conversely, aerosol cloud processing can affect the morphology and mixing of the particles. For example, fresh soot has typically an open fractal-like structure, but aging and cloud processing can restructure soot into more compacted shapes, with different optical and ice nucleation properties. During my graduate research, I used an array of electron microscopy and image analysis tools to study morphology and mixing state of a large number of individual particles collected during several field and laboratory studies. To this end, I investigated various types of particles such as tar balls (spherical carbonaceous particles emitted during biomass burning) and dust particles, but with a special emphasis on soot particles. In addition, I used the Stony Brook ice nucleation cell facility to investigate heterogeneous ice nucleation and water uptake by long-range transported particles collected at the Pico Mountain Observatory, in the Archipelago of the Azores. Finally, I used ice nucleation data from the SAAS (Soot Aerosol Aging Study) chamber study at the Pacific Northwest National Laboratory to understand the effects that ice nucleation and supercooled water processing has on the morphology of residual soot particles. Some highlights of our findings and implications are discussed next. We found that the morphology of fresh soot emitted by vehicles depends on the driving conditions (i.e.; the vehicle specific power). Soot emitted by biomass burning is often heavily coated by other materials while processing of soot in urban environment exhibits complex mixing. We also found that long-range transported soot over the ocean after atmospheric processing is very compacted. In addition, our results suggest that freezing process can facilitate restructuring of soot and results into collapsed soot. Furthermore, numerical simulations showed strong influence on optical properties when fresh open fractal-like soot evolved to collapsed soot. Further investigation of long-range transported aged particles exhibits that they are efficient in water uptake and can induce ice nucleation in colder temperature. Our results have implications for assessing the impact of the morphology and mixing state of soot particles on human health, environment and climate. Our findings can provide guidance to numerical models such as particle-resolved mixing state models to account for, and better understand, vehicular emissions and soot evolution since its emission to atmospheric processing in urban environment and finally in remote regions after long-range transport. Morphology and mixing state information can be used to model observational-constrained optical properties. The details of morphology and mixing state of soot particles are crucial to assess the accuracy of climate models in describing the contribution of soot radiative forcing and their direct and indirect climate effects. Finally, our observations of ice nucleation ability by aged particles show that nucleated particles are internally mixed and coated with several materials.

Analysis of large oxygenated and nitrated polycyclic aromatic hydrocarbons formed under simulated diesel engine exhaust conditions (by compound fingerprints with SPE/LC-API-MS)

PubMed Central

Adelhelm, Christoph; Niessner, Reinhard; Pöschl, Ulrich

2008-01-01

The analysis of organic compounds in combustion exhaust particles and the chemical transformation of soot by nitrogen oxides are key aspects of assessment and mitigation of the climate and health effects of aerosol emissions from fossil fuel combustion and biomass burning. In this study we present experimental and analytical techniques for efficient investigation of oxygenated and nitrated derivatives of large polycyclic aromatic hydrocarbons (PAHs), which can be regarded as well-defined soot model substances. For coronene and hexabenzocoronene exposed to nitrogen dioxide under simulated diesel exhaust conditions, several reaction products with high molecular mass could be characterized by liquid chromatography-atmospheric pressure chemical (and photo) ionization-mass spectrometry (LC-APCI-MS and LC-APPI-MS). The main products of coronene contained odd numbers of nitrogen atoms (m/z 282, 256, 338), whereas one of the main products of hexabenzocoronene exhibited an even number of nitrogen atoms (m/z 391). Various reaction products containing carbonyl and nitro groups could be tentatively identified by combining chromatographic and mass spectrometric information, and changes of their relative abundance were observed to depend on the reaction conditions. This analytical strategy should highlight a relatively young technique for the characterization of various soot-contained, semi-volatile, and semi-polar reaction products of large PAHs. Figure LC-APCI-MS analysis of nitrated coronene (and HBC): Total-Ion-Chromatogram (TIC), Extracted Ion Chromatograms (EICs) and corresponding mass spectrum (top). PMID:18560812

Laminar soot processes

NASA Technical Reports Server (NTRS)

Sunderland, P. B.; Lin, K.-C.; Faeth, G. M.

1995-01-01

Soot processes within hydrocarbon fueled flames are important because they affect the durability and performance of propulsion systems, the hazards of unwanted fires, the pollutant and particulate emissions from combustion processes, and the potential for developing computational combustion. Motivated by these observations, the present investigation is studying soot processes in laminar diffusion and premixed flames in order to better understand the soot and thermal radiation emissions of luminous flames. Laminar flames are being studied due to their experimental and computational tractability, noting the relevance of such results to practical turbulent flames through the laminar flamelet concept. Weakly-buoyant and nonbuoyant laminar diffusion flames are being considered because buoyancy affects soot processes in flames while most practical flames involve negligible effects of buoyancy. Thus, low-pressure weakly-buoyant flames are being observed during ground-based experiments while near atmospheric pressure nonbuoyant flames will be observed during space flight experiments at microgravity. Finally, premixed laminar flames also are being considered in order to observe some aspects of soot formation for simpler flame conditions than diffusion flames. The main emphasis of current work has been on measurements of soot nucleation and growth in laminar diffusion and premixed flames.

Structure and Soot Properties of Nonbuoyant Ethylene/Air Laminar Jet Diffusion Flames. Appendix E; Repr. from AIAA Journal, v. 36 p 1346-1360

NASA Technical Reports Server (NTRS)

Urban, D. L.; Yuan, Z.-G.; Sunderland, P. B.; Linteris, G. T.; Voss, J. E.; Lin, K.-C.; Dai, Z.; Sun, K.; Faeth, G. M.; Ross, Howard D. (Technical Monitor)

2001-01-01

The structure and soot properties of round, soot-emitting, nonbuoyant, laminar jet diffusion flames are described, based on long-duration (175-230-s) experiments at microgravity carried out on orbit in the Space Shuttle Columbia. Experimental conditions included ethylene-fueled flames burning in still air at nominal pressures of 50 and 100 kPa and an ambient temperature of 300 K with luminous flame lengths of 49-64 mm Measurements included luminous flame shapes using color video imaging soot concentration (volume fraction) distributions using deconvoluted laser extinction imaging, soot temperature distributions using deconvoluted multiline emission imaging, gas temperature distributions at fuel-lean (plume) conditions using thermocouple probes, soot structure distributions using thermophoretic sampling and analysis by transmission electron microscopy, and flame radiation using a radiometer.The present flames were larger, and emitted soot more readily, than comparable flames observed during ground-based microgravity experiments due to closer approach to steady conditions resulting from the longer test times and the reduced gravitational disturbances of the space-based experiments.

Grand canonical Monte Carlo simulation of the adsorption isotherms of water molecules on model soot particles

NASA Astrophysics Data System (ADS)

Moulin, F.; Picaud, S.; Hoang, P. N. M.; Jedlovszky, P.

2007-10-01

The grand canonical Monte Carlo method is used to simulate the adsorption isotherms of water molecules on different types of model soot particles. The soot particles are modeled by graphite-type layers arranged in an onionlike structure that contains randomly distributed hydrophilic sites, such as OH and COOH groups. The calculated water adsorption isotherm at 298K exhibits different characteristic shapes depending both on the type and the location of the hydrophilic sites and also on the size of the pores inside the soot particle. The different shapes of the adsorption isotherms result from different ways of water aggregation in or/and around the soot particle. The present results show the very weak influence of the OH sites on the water adsorption process when compared to the COOH sites. The results of these simulations can help in interpreting the experimental isotherms of water adsorbed on aircraft soot.

Source Estimation of Wintertime Soot Particles for an Urban Site Varanasi (25.30 N, 83.00 E) in Central Indo-Gangetic Plain Region

NASA Astrophysics Data System (ADS)

Singh, A. K.; Srivastava, M. K.; Dumka, U. C.; Singh, R. K.; Singh, R. S.; Tiwari, S.; Mehrotra, B. J.; Srivastava, A. K.

2017-12-01

Black carbon particles (BC: also called Soot) are formed by incomplete combustion of hydrocarbon based fuels (fossil fuel: coal, diesel, petrol, etc.) as well as due to burning of biomass and bio-fuels (wood, shrubs, dry leaves, etc.). Soot particles are warming agent to the atmosphere that gained wide attention in recent years due to their direct and indirect impacts on local, regional as well as global climate. The climatic effects due to soot are not well understood as indicated by large uncertainties in their climate forcing estimation, particularly in South and East Asian region, possibly due to unavailability of adequate database and information about the source. Measurement of wintertime BC mass concentrations for urban site in central IGP, `Varanasi' (25.30 N, 83.00 E), using a seven wavelength Aethalometer is reported in this work. Delta-C (=BC370 - BC880), which is an indicator of biomass/bio-fuels or residential coal burning is used to understand the source. Aethalometer based source apportionment model "Aethalometer model" was used to apportion the fossil fuel/traffic and wood/biomass burning mass concentration to the total BC mass. The preliminary results for representative month (January-2015) show that daily-average BC mass ranged from 4.47 to 20.70 μg m-3 (Average: 9.45 ± 4.15 μg m-3). The daily Absorption Ångström Exponent (AAE) and the ratio of BCff/BC and BCff/BCwb varied between 1.09 - 1.32, 0.67 - 0.92 and 2 - 40, respectively, due to the changes in BC emissions rates. The total BC, BC from fossil fuel (BCff) and BC from wood/biomass burning (BCwb) behaved in the remarkable diurnal pattern, behaving opposite to the mixing layer heights (MLHs). During daytime, MLHs are higher due to surface based solar warming and causes more volume of atmosphere for the BC dispersion. This phenomenon causes the surface measurement of lower BC mass during the daytime. The data is, however, still being processed for multi-year wintertime observations and the detailed discussions will be shown during the presentation.

Ozone as a Sink for Atmospheric Carbon Aerosols

NASA Astrophysics Data System (ADS)

Stephens, Sherry Lynn

Critical information necessary for examining the chemical removal of smoke in the atmosphere by the reaction with ozone has been obtained. The kinetics, products and temperature dependence of the reaction of ozone with carbonaceous material were determined. This information can be included in models examining the fate of ozone and smoke in the atmosphere. In the first study, the rate of ozone loss was followed in its reaction with carbon black at room temperature. In addition to the ozone loss, the gaseous products, CO, CO _2 and O_2 were quantified with a phase locking mass spectrometer attached to a two-chamber Knudsen cell reactor. An oxygen molecule was detected for every ozone lost. It was observed that the initial loss rate was much greater than that seen after extended exposure to ozone. Oxygen atoms were desorbed 30% of the time as CO or CO_2 and those left behind on the surface were responsible for the decrease in rate. Heating the surface following this exposure would liberate CO and CO_2 and restore the initial reactivity. In the second study, the reaction of ozone with different types of soot was examined by following the decrease of optical depth of soot deposited on a quartz slide as a result of flowing a known concentration of ozone over the slide at temperatures from 21^circ to 175^circC. The reaction kinetics were very similar for the four types of soot used in this study. Treating all types together the activation energy and the order with respect to ozone were 10.9 (+/-1.0) kcal mol ^{-1} and 0.89 (+/- 0.14), respectively. The lifetime of soot under atmospheric conditions was calculated to be on the order of years to decades. The reaction of ozone with acetylene smoke suspended in air was the final method of examining the reaction. The change of acetylene smoke size distribution and ozone concentration was monitored while controlling the temperature. Irreproducibility caused this study to be unsuccessful. This was believed to be due to contamination leaking into the teflon bags in which the experiments were conducted. Several attempts to alleviate this problem were unsuccessful.

Fullerene Soot in Eastern China Air: Results from Soot Particle-Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Wang, J.; Ge, X.; Chen, M.; Zhang, Q.; Yu, H.; Sun, Y.; Worsnop, D. R.; Collier, S.

2015-12-01

In this work, we present for the first time, the observation and quantification of fullerenes in ambient airborne particulate using an Aerodyne Soot Particle - Aerosol Mass Spectrometer (SP-AMS) deployed during 2015 winter in suburban Nanjing, a megacity in eastern China. The laser desorption and electron impact ionization techniques employed by the SP-AMS allow us to differentiate various fullerenes from other aerosol components. Mass spectrum of the identified fullerene soot is consisted by a series of high molecular weight carbon clusters (up to m/z of 2000 in this study), almost identical to the spectral features of commercially available fullerene soot, both with C70 and C60 clusters as the first and second most abundant species. This type of soot was observed throughout the entire study period, with an average mass loading of 0.18 μg/m3, accounting for 6.4% of the black carbon mass, 1.2% of the total organic mass. Temporal variation and diurnal pattern of fullerene soot are overall similar to those of black carbon, but are clearly different in some periods. Combining the positive matrix factorization, back-trajectory and analyses of the meteorological parameters, we identified the petrochemical industrial plants situating upwind from the sampling site, as the major source of fullerene soot. In this regard, our findings imply the ubiquitous presence of fullerene soot in ambient air of industry-influenced area, especially the oil and gas production regions. This study also offers new insights into the characterization of fullerenes from other environmental samples via the advanced SP-AMS technique.

Microgravity

NASA Image and Video Library

1999-01-01

Gerard M. Faeth, University of Michigan, principal investigator in combustion science experiments, including Flow/Soot-Formation in Nonbuoyant Laminar Diffusion Flames, investigation of Laminar Jet Diffusion Flames in Microgravity: A Paradigm for Soot Processes in Turbulent Flames, and Soot Processes in Freely-Propagating Laminar Premixed Flames.

Soot blower using fuel gas as blowing medium

DOEpatents

Tanca, Michael C.

1982-01-01

A soot blower assembly (10) for use in combination with a coal gasifier (14). The soot blower assembly is adapted for use in the hot combustible product gas generated in the gasifier as the blowing medium. The soot blower lance (20) and the drive means (30) by which it is moved into and out of the gasifier is housed in a gas tight enclosure (40) which completely surrounds the combination. The interior of the enclosure (40) is pressurized by an inert gas to a pressure level higher than that present in the gasifier so that any combustible product gas leaking from the soot blower lance (20) is forced into the gasifier rather than accumulating within the enclosure.

Rapid Response Research and Development (R&D) for the Aerospace Systems Directorate. Delivery Order 0021: Engineering Research and Technical Analyses of Advanced Airbreathing Propulsion Fuels, Subtask: Engine and Pump Studies Utilizing JP-8 and Alcohol-to-Jet (ATJ) Blends

DTIC Science & Technology

2014-08-01

41 Figure A-21. Lubricant Soot Accumulation...ASTM D4739 Total Base Number ASTM D664 Total Acid Number ASTM D445 Kinematic Viscosity @ 100°C ASTM D4052 Density ASTM TGA SOOT TGA Soot ASTM E168...118.85 134.01 145.47 169.22 187.43 342.42 Nitration (Abs./cm) E168 FTIR 0 6.67 10.91 16.54 19.04 25.79 35.12 24.03 23.75 52.31 93.9 Soot (%) Soot TGA

A Method for Eliminating Beam Steering Error for the Modulated Absorption-Emission Thermometry Technique

DTIC Science & Technology

2014-01-01

broadened and merged. It is also suitable for environments where broadband emitters such as soot are present. Radiometric measurements in general can be...emitters such as soot are present. Radiometric measurements in general can be made with very high accuracy. The international temperature scale (ITS...by a fitting to a model. In the case of sooting flames, the emissivity is a result of the nearly black absorption and emission features of soot

Precursor soot synthesis of fullerenes and nanotubes without formation of carbonaceous soot

DOEpatents

Reilly, Peter T. A.

2007-03-20

The present invention is a method for the synthesis of fullerenes and/or nanotubes from precursor soot without the formation of carbonaceous soot. The method comprises the pyrolysis of a hydrocarbon fuel source by heating the fuel source at a sufficient temperature to transform the fuel source to a condensed hydrocarbon. The condensed hydrocarbon is a reaction medium comprising precursor soot wherein hydrogen exchange occurs within the reaction medium to form reactive radicals which cause continuous rearrangement of the carbon skeletal structure of the condensed hydrocarbon. Then, inducing dehydrogenation of the precursor soot to form fullerenes and/or nanotubes free from the formation of carbonaceous soot by continued heating at the sufficient temperature and by regulating the carbon to hydrogen ratio within the reaction medium. The dehydrogenation process produces hydrogen gas as a by-product. The method of the present invention in another embodiment is also a continuous synthesis process having a continuous supply of the fuel source. The method of the present invention can also be a continuous cyclic synthesis process wherein the reaction medium is fed back into the system as a fuel source after extraction of the fullerenes and/or nanotube products. The method of the present invention is also a method for producing precursor soot in bulk quantity, then forming fullerenes and/or nanotubes from the precursor bulk.

Tackling a Hot Paradox: Laminar Soot Processes-2 (LSP-2)

NASA Technical Reports Server (NTRS)

Faeth, Gerard M.; Urban, David L.; Over, Ann (Technical Monitor)

2002-01-01

The last place you want to be in traffic is behind the bus or truck that is belching large clouds of soot onto your freshly washed car. Besides looking and smelling bad, soot is a health hazard. Particles range from big enough to see to microscopic and can accumulate in the lungs, potentially leading to debilitating or fatal lung diseases. Soot is wasted energy, and therein lies an interesting paradox: Soot forms in a flame's hottest regions where you would expect complete combustion and no waste. Soot enhances the emissions of other pollutants (carbon monoxide and polyaromatic hydrocarbons, etc.) from flames and radiates unwanted heat to combustion chambers (a candle's yellowish glow is soot radiating heat), among other effects. The mechanisms of soot formation are among the most important unresolved problems of combustion science because soot affects contemporary life in so many ways. Although we have used fire for centuries, many fundamental aspects of combustion remain elusive, in part because of limits imposed by the effects of gravity on Earth. Hot or warm air rises quickly and draws in fresh cold air behind it, thus giving flames the classical teardrop shape. Reactions occur in a very small zone, too fast for scientists to observe, in detail, what is happening inside the flame. The Laminar Soot Processes (LSP-2) experiments aboard STS-107 will use the microgravity environment of space to eliminate buoyancy effects and thus slow the reactions inside a flame so they can be more readily studied. 'Laminar' means a simple, smooth fuel jet burning in air, somewhat like a butane lighter. This classical flame approximates combustion in diesel engines, aircraft jet propulsion engines, and furnaces and other devices. LSP-2 will expand on surprising results developed from its first two flights in 1997. The data suggest the existence of a universal relationship, the soot paradigm, that, if proven, will be used to model and control combustion systems on Earth. STS-107 experiments also will help set the stage for extended combustion experiments aboard the International Space Station.

Structure of the Soot Growth Region of Laminar Premixer Methane/Oxygen Flames

NASA Technical Reports Server (NTRS)

Xu, F.; Faeth, G. M.

1999-01-01

Soot is a dominant feature of hydrocarbon/air flames, affecting their reaction mechanisms and structure. As a result, soot processes affect capabilities for computational combustion as well as predictions of flame radiation and pollution emissions. Motivated by these observations, the present investigation extended past work on soot growth in laminar premixed flames, seeking to evaluate model predictions of flame structure. Xu et al. report direct measurements of soot residence times, soot concentrations, soot structure, gas temperatures and gas compositions for premixed flames similar to those studied by Harris and Weiner and Ramer et al. respectively. It was found that predictions of major stable gas species concentrations based on mechanisms of Leung and Lindstedt and Frenklach and coworkers, were in good agreement with the measurements. The results were also used to evaluate the hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms of Frenklach and coworkers and Colket and Hall. It was found that these mechanisms were effective using quite reasonable correlations for the steric factors appearing in the theories. The successful evaluation of the HACA mechanism of soot growth in Refs. 1 and 2 is encouraging but one aspect of this evaluation is a concern. In particular, H-atom concentrations play a crucial role in the HACA mechanism and it was necessary to estimate these concentrations because they were not measured directly. These estimates were made assuming local thermodynamic equilibrium between H, and H based on measured temperatures and H2 concentrations and the equilibrium constant data of Kee et al.. This approach was justified by the flame structure predictions; nevertheless, direct evaluation of equilibrium estimates of H-atom concentrations in the soot growth regions of laminar premixed flames is needed to provide more convincing proof of this behavior. Thus, the objective of the present investigation was to complete new measurements of the structure of the soot growth region of laminar premixed flames and to use these results to evaluate whether H and H2 are in thermodynamic equilibrium and to extend the earlier evaluation of predictions of concentrations of major gas species.

The competition between mineral dust and soot ice nuclei in mixed-phase clouds (Invited)

NASA Astrophysics Data System (ADS)

Murray, B. J.; Atkinson, J.; Umo, N.; Browse, J.; Woodhouse, M. T.; Whale, T.; Baustian, K. J.; Carslaw, K. S.; Dobbie, S.; O'Sullivan, D.; Malkin, T. L.

2013-12-01

The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. In this talk our recent laboratory and global aerosol modelling work on mineral dust and soot ice nuclei will be presented. We have performed immersion mode experiments to quantify ice nucleation by the individual minerals which make up desert mineral dusts and have shown that the feldspar component, rather than the clay component, is most important for ice nucleation (Atkinson et al. 2013). Experiments with well-characterised soot generated with eugenol, an intermediate in biomass burning, and n-decane show soot has a significant ice nucleation activity in mixed-phase cloud conditions. Our results for soot are in good agreement with previous results for acetylene soot (DeMott, 1990), but extend the efficiency to much higher temperatures. We then use a global aerosol model (GLOMAP) to map the distribution of soot and feldspar particles on a global basis. We show that below about -15oC that dust and soot together can explain most observed ice nuclei in the Earth's atmosphere, while at warmer temperatures other ice nuclei types are needed. We show that in some regions soot is the most important ice nuclei (below -15oC), while in others feldspar dust dominates. Our results suggest that there is a strong anthropogenic contribution to the ice nuclei population, since a large proportion of soot aerosol in the atmosphere results from human activities. Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Carslaw, K. S., Whale, T. F., Baustian, K. J., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 10.1038/nature12278, (2013). Demott, P. J. 1990. An Exploratory-Study of Ice Nucleation by Soot Aerosols. Journal of Applied Meteorology, 29, 1072-1079.

Carbon-catalyzed oxidation of SO2 by NO2 and air

NASA Technical Reports Server (NTRS)

Rogowski, R. S.; Schryer, D. R.; Cofer, W. R., III; Edahl, R. A., Jr.; Munavalli, S.

1982-01-01

A series of experiments was performed using carbon particles (commercial furnace black) as a surrogate for soot particles. Carbon particles were suspended in water, and gas mixtures were bubbled into the suspensions to observe the effect of carbon particles on the oxidation of SO2 by air and NO2. Identical gas mixtures were bubbled into a blank containing only pure water. After exposure each solution was analyzed for pH and sulfate. It was found that NO2 greatly enhances the oxidation of SO2 to sulfate in the presence of carbon particles. The amount of sulfate found in the blanks was significantly less. Under the conditions of these experiments no saturation of the reaction was observed and SO2 was converted to sulfate even in a highly acid medium (pH or = 1.5).

Oxidation of SO2 by NO2 and air in an aqueous suspension of carbon

NASA Technical Reports Server (NTRS)

Rogowski, R. S.; Schryer, D. R.; Cofer, W. R., III; Edahl, R. A., Jr.; Munavalli, S.

1982-01-01

A series of experiments has been performed using carbon black as a surrogate for soot particles. Carbon black was suspended in water and gas mixtures were bubbled into the suspensions to observe the effect of carbon particles on the oxidation of SO2 by air and NO2. Identical gas mixtures were bubbled into a black containing only pure water. After exposure each solution was analyzed for pH and sulfate. It was found that NO2 greatly enhances the oxidation of SO2 to sulfate in the presence of carbon black. The amount of sulfate in the blanks was significantly less. Under the conditions of the experiments no saturation of the reaction was observed and SO2 was converted to sulfate even in a highly acid medium (pH not less than 1.5).

Soot

Cancer.gov

Learn about soot, which can raise the risk of scrotal and other skin cancers, as well as lung, esophageal, and bladder cancers. Soot is a byproduct of the burning of carbon-containing materials, such as wood, fuel oil, plastics, and household refuse. Chimney sweeps face the highest risk.

Combustor for fine particulate coal

DOEpatents

Carlson, L.W.

1988-01-26

A particulate coal combustor with two combustion chambers is provided. The first combustion chamber is toroidal; air and fuel are injected, mixed, circulated and partially combusted. The air to fuel ratio is controlled to avoid production of soot or nitrogen oxides. The mixture is then moved to a second combustion chamber by injection of additional air where combustion is completed and ash removed. Temperature in the second chamber is controlled by cooling and gas mixing. The clean stream of hot gas is then delivered to a prime mover. 4 figs.

Combustor for fine particulate coal

DOEpatents

Carlson, Larry W.

1988-01-01

A particulate coal combustor with two combustion chambers is provided. The first combustion chamber is toroidal; air and fuel are injected, mixed, circulated and partially combusted. The air to fuel ratio is controlled to avoid production of soot or nitrogen oxides. The mixture is then moved to a second combustion chamber by injection of additional air where combustion is completed and ash removed. Temperature in the second chamber is controlled by cooling and gas mixing. The clean stream of hot gas is then delivered to a prime mover.

Experimental Study of the Oxidation, Ignition, and Soot Formation Characteristics of Jet Fuel

DTIC Science & Technology

2010-09-29

section and controls the heat flux applied to six heated zones along the 4.11 m long driven section, and 2.5 cm thick mineral wool insulation that...The mixing manifold was insulated with 1.1 cm thick silicon foam rubber insulation, and the mixing vessel was insulated with 2.5 cm- thick mineral ... wool insulation. Experimental work for a number of compounds with variation in manifold and tank heating showed no observable difference in measured

Combustor for fine particulate coal

DOEpatents

Carlson, L.W.

1988-11-08

A particulate coal combustor with two combustion chambers is provided. The first combustion chamber is toroidal; air and fuel are injected, mixed, circulated and partially combusted. The air to fuel ratio is controlled to avoid production of soot or nitrogen oxides. The mixture is then moved to a second combustion chamber by injection of additional air where combustion is completed and ash removed. Temperature in the second chamber is controlled by cooling and gas mixing. The clean stream of hot gas is then delivered to a prime mover. 4 figs.

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

NASA Astrophysics Data System (ADS)

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.

An Experimental and Computational Study on Soot Formation in a Coflow Jet Flame Under Microgravity and Normal Gravity

NASA Technical Reports Server (NTRS)

Ma, Bin; Cao, Su; Giassi, Davide; Stocker, Dennis P.; Takahashi, Fumiaki; Bennett, Beth Anne V.; Smooke, Mitchell D.; Long, Marshall B.

2014-01-01

Upon the completion of the Structure and Liftoff in Combustion Experiment (SLICE) in March 2012, a comprehensive and unique set of microgravity coflow diffusion flame data was obtained. This data covers a range of conditions from weak flames near extinction to strong, highly sooting flames, and enabled the study of gravitational effects on phenomena such as liftoff, blowout and soot formation. The microgravity experiment was carried out in the Microgravity Science Glovebox (MSG) on board the International Space Station (ISS), while the normal gravity experiment was performed at Yale utilizing a copy of the flight hardware. Computational simulations of microgravity and normal gravity flames were also carried out to facilitate understanding of the experimental observations. This paper focuses on the different sooting behaviors of CH4 coflow jet flames in microgravity and normal gravity. The unique set of data serves as an excellent test case for developing more accurate computational models.Experimentally, the flame shape and size, lift-off height, and soot temperature were determined from line-of-sight flame emission images taken with a color digital camera. Soot volume fraction was determined by performing an absolute light calibration using the incandescence from a flame-heated thermocouple. Computationally, the MC-Smooth vorticity-velocity formulation was employed to describe the chemically reacting flow, and the soot evolution was modeled by the sectional aerosol equations. The governing equations and boundary conditions were discretized on an axisymmetric computational domain by finite differences, and the resulting system of fully coupled, highly nonlinear equations was solved by a damped, modified Newtons method. The microgravity sooting flames were found to have lower soot temperatures and higher volume fraction than their normal gravity counterparts. The soot distribution tends to shift from the centerline of the flame to the wings from normal gravity to microgravity.

Planar measurements of soot volume fraction and OH in a JP-8 pool fire

DOE Office of Scientific and Technical Information (OSTI.GOV)

Henriksen, Tara L.; Ring, Terry A.; Eddings, Eric G.

2009-07-15

The simultaneous measurement of soot volume fraction by laser induced incandescence (LII) and qualitative imaging of OH by laser induced fluorescence (LIF) was performed in a JP-8 pool fire contained in a 152 mm diameter pan. Line of sight extinction was used to calibrate the LII system in a laminar flame, and to provide an independent method of measuring average soot volume fraction in the turbulent flame. The presence of soot in the turbulent flame was found to be approximately 50% probable, resulting in high levels of optical extinction, which increased slightly through the flame from approximately 30% near themore » base, to approximately 50% at the tip. This high soot loading pushes both techniques toward their detection limit. Nevertheless, useful accuracy was obtained, with the LII measurement of apparent extinction in the turbulent flame being approximately 21% lower than a direct measurement, consistent with the influence of signal trapping. The axial and radial distributions of soot volume fraction are presented, along with PDFs of volume fraction, and new insight into the behavior of soot sheets in pool fires are sought from the simultaneous measurements of OH and LII. (author)« less

Aviation Fuel Tracer Simulation: Model Intercomparison and Implications

NASA Technical Reports Server (NTRS)

Danilin, M. Y.; Fahey, D. W.; Schumann, U.; Prather, M. J.; Penner, J. E.; Ko, M. K. W.; Weisenstein, D. K.; Jackman, C. H.; Pitari, G.; Koehler, I.;

Aviation Fuel Tracer Simulation: Model Intercomparison and Implications

NASA Technical Reports Server (NTRS)

Danilin, M. Y.; Fahey, D. W.; Schumann, U.; Prather, M. J.; Penner, J. E.; Ko, M. K. W.; Weisenstein, D. K.; Jackman, C. H.; Pitari, G.; Koehler, I.;

The Impact of Buoyancy and Flame Structure on Soot, Radiation and NOx Emissions from a Turbulent Diffusion Flame

NASA Technical Reports Server (NTRS)

Kennedy, I. M.; Kollman, W.; VanderWal, R. L.

1999-01-01

It is hypothesized that the spatial structure of a turbulent diffusion flame plays an important role in determining the emissions of radiative energy, soot and NO, from a combustor. This structure, manifested in the two point statistics, is influenced by buoyancy. Radiation, soot and NOx emissions are the cumulative result of processes that occur throughout a flame. For example, radiation fluxes along a line of sight can be found from summing up the contributions from sources in individual pockets of hot soot that emit, and from sinks in cold soot that absorb. Soot and NOx are both the results of slow chemistry and are not equilibrium products. The time that is available for production and burnout is crucial in determining the eventual emissions of these pollutants. Turbulence models generally rely on a single point closure of the appropriate time averaged equations. Hence, spatial information is lost and needs to be modeled using solution variables such as turbulence kinetic energy and dissipation rate, often with the assumption of isotropy. However, buoyancy can affect the physical structure of turbulent flames and can change the spatial extent of soot bearing regions. Theoretical comparisons with models are best done in the limit of infinite Froude number because the inclusion of buoyancy in flow models introduces significant uncertainties. Hence, LII measurements of soot, measurements of radiation fluxes from soot, Particle Imaging Velocimetry (PIV) of the flow field and measurements of post flame NOX will be carried out on the NASA Lewis 2.2 sec drop tower and eventually on the parabolic flight aircraft. The drop rig will be a modified version of a unit that has been successfully used at Lewis in the past.

Sooting Limits Of Diffusion Flames With Oxygen-Enriched Air And Diluted Fuel

NASA Technical Reports Server (NTRS)

Sunderland, P. B.; Urban, D. L.; Stocker, D. P.; Chao, B. H.; Axelbaum, R. L.

2003-01-01

Oxygen-enhanced combustion permits certain benefits and flexibility that are not otherwise available in the design of practical combustors, as discussed by Baukal. The cost of pure and enriched oxygen has declined to the point that oxygen-enhanced combustion is preferable to combustion in air for many applications. Carbon sequestration is greatly facilitated by oxygen enrichment because nitrogen can be eliminated from the product stream. For example, when natural gas (or natural gas diluted with CO2) is burned in pure oxygen, the only significant products are water and CO2. Oxygen-enhanced combustion also has important implications for soot formation, as explored in this work. We propose that soot inception in nonpremixed flames requires a region where C/O ratio, temperature, and residence time are above certain critical values. Soot does not form at low temperatures, with the threshold in nonpremixed flames ranging from about 1250-1650 K, a temperature referred to here as the critical temperature for soot inception, Tc. Soot inception also can be suppressed when residence time is short (equivalently, when the strain rate in counterflow flames is high). Soot induction times of 0.8-15 ms were reported by Tesner and Shurupov for acetylene/nitrogen mixtures at 1473 K. Burner stabilized spherical microgravity flames are employed in this work for two main reasons. First, this configuration offers unrestricted control over convection direction. Second, in steady state these flames are strain-free and thus can yield intrinsic sooting limits in diffusion flames, similar to the way past work in premixed flames has provided intrinsic values of C/O ratio associated with soot inception limits.

Measurements of Soot Mass Absorption Coefficients from 300 to 660 nm

NASA Astrophysics Data System (ADS)

Renbaum-Wolff, Lindsay; Fisher, Al; Helgestad, Taylor; Lambe, Andrew; Sedlacek, Arthur; Smith, Geoffrey; Cappa, Christopher; Davidovits, Paul; Onasch, Timothy; Freedman, Andrew

2016-04-01

Soot, a product of incomplete combustion, plays an important role in the earth's climate system through the absorption and scattering of solar radiation. In particular, the assumed mass absorption coefficient (MAC) of soot and its variation with wavelength presents a significant uncertainty in the calculation of radiative forcing in global climate change models. As part of the fourth Boston College/Aerodyne soot properties measurement campaign, we have measured the mass absorption coefficient of soot produced by an inverted methane diffusion flame over a spectral range of 300-660 nm using a variety of optical absorption techniques. Extinction and absorption were measured using a dual cavity ringdown photoacoustic spectrometer (CRD-PAS, UC Davis) at 405 nm and 532 nm. Scattering and extinction were measured using a CAPS PMssa single scattering albedo monitor (Aerodyne) at 630 nm; the absorption coefficient was determined by subtraction. In addition, the absorption coefficients in 8 wavelength bands from 300 to 660 nm were measured using a new broadband photoacoustic absorption monitor (UGA). Soot particle mass was quantified using a centrifugal particle mass analyzer (CPMA, Cambustion), mobility size with a scanning mobility particle sizer (SMPS, TSI) and soot concentration with a CPC (Brechtel). The contribution of doubly charged particles to the sample mass was determined using a Single Particle Soot Photometer (DMT). Over a mass range of 1-8 fg, corresponding to differential mobility diameters of ~150 nm to 550 nm, the value of the soot MAC proved to be independent of mass for all wavelengths. The wavelength dependence of the MAC was best fit to a power law with an Absorption Ångstrom Coefficient slightly greater than 1.

Albedo and flux extinction coefficient of impure snow for diffuse shortwave radiation

NASA Technical Reports Server (NTRS)

Choudhury, B. J.; Mo, T.; Wang, J. R.; Chang, A. T. C.

1981-01-01

Impurities enter a snowpack as a result of fallout of scavenging by falling snow crystals. Albedo and flux extinction coefficient of soot contaminated snowcovers were studied using a two stream approximation of the radiative transfer equation. The effect of soot was calculated by two methods: independent scattering by ice grains and impurities and average refractive index for ice grains. Both methods predict a qualitatively similar effect of soot; the albedo is decreased and the extinction coefficient is increased compared to that for pure snow in the visible region; the infrared properties are largely unaffected. Quantitatively, however, the effect of soot is more pronounced in the average refractive index method. Soot contamination provides a qualitative explanation for several snow observations.

Soot formation in the methane oxygen and methane/oxygen/hydrogen flame

NASA Technical Reports Server (NTRS)

Dauerman, L.; Salser, G. E.

1972-01-01

The feasibility of using methane, recovered from carbon dioxide by the Sabatier-Senderens reaction, was investigated as a fuel in a reaction control engine. A problem to be avoided is the emission of soot particles. It is thought that such particles would remain in the environment of the spacecraft and, thereby, adversely affect optical sightings and possibly have an effect upon communications. The initial studies were of a practical nature. The first was the influence of the spatial arrangement of the fuel and oxygen injectors on soot formation. In the second study, inhibition of soot formation was considered. Considering the given situation, it was impractical to use an additive. However, since methanol combustion does not produce soot, and methanol can be produced from methane in situ, the possibility that methanol could act as an inhibitor was studied. In the third study, since these are restartable engines, the effect of shutdown on the rapidity of soot formation was studied.

Determination of polycyclic aromatic hydrocarbons in kerosene and bio-kerosene soot.

PubMed

Andrade-Eiroa, Auréa; Leroy, Valérie; Dagaut, Philippe; Bedjanian, Yuri

2010-03-01

Here we report a new, efficient and reliable analytical methodology for sensitive and selective quantification of Polycyclic Aromatic Hydrocarbons (PAHs) in soot samples. The methodology developed is based on ultrasonic extraction of the soot-bound PAHs into small volumes of acetonitrile, purification of the extracts through C(18) Solid Phase Extraction (SPE) cartridges and analysis by Reverse Phase Liquid Chromatography (RPLC) with UV and fluorimetric detection. For the first time, we report the convenience of adapting the SPE procedure to the nature of the soot samples. As a matter of fact, extracts containing high percentage of unpolar material are recommended to be cleaned with acetone, whereas extracts poor in unpolar compounds can be efficiently cleaned with methanol. The method was satisfactorily applied to kerosene and bio-kerosene soot from atmospheric open diffusion flames (pool fires) and premixed flames achieving Quantification and Detection limits in the range ng mg(-1) soot and recoveries about 90% for most of the PAHs studied. Copyright (c) 2010 Elsevier Ltd. All rights reserved.

Structure and Soot Properties of Nonbuoyant Ethylene/Air Laminar Jet Diffusion Flames. Appendix I

NASA Technical Reports Server (NTRS)

Urban, D. L.; Yuan, Z.-G.; Sunderland, P. B.; Linteris, G. T.; Voss, J. E.; Lin, K.-C.; Dai, Z.; Sun, K.; Faeth, G. M.; Ross, Howard D. (Technical Monitor)

2000-01-01

The structure and soot properties of round, soot-emitting, nonbuoyant, laminar jet diffusion flames are described, based on long-duration (175-230/s) experiments at microgravity carried out on orbit In the Space Shuttle Columbia. Experiments] conditions included ethylene-fueled flames burning in still air at nominal pressures of 50 and 100 kPa and an ambient temperature of 300 K with luminous Annie lengths of 49-64 mm. Measurements included luminous flame shapes using color video imaging, soot concentration (volume fraction) distributions using deconvoluted laser extinction imaging, soot temperature distributions using deconvoluted multiline emission imaging, gas temperature distributions at fuel-lean (plume) conditions using thermocouple probes, not structure distributions using thermophoretic sampling and analysis by transmission electron microscopy, and flame radiation using a radiometer. The present flames were larger, and emitted soot men readily, than comparable observed during ground-based microgravity experiments due to closer approach to steady conditions resulting from the longer test times and the reduced gravitational disturbances of the space-based experiments.

Detailed modeling analysis for soot formation and radiation in microgravity gas jet diffusion flames

NASA Technical Reports Server (NTRS)

Ku, Jerry C.; Tong, LI; Greenberg, Paul S.

1995-01-01

Radiation heat transfer in combustion systems has been receiving increasing interest. In the case of hydrocarbon fuels, a significant portion of the radiation comes from soot particles, justifying the need for detailed soot formation model and radiation transfer calculations. For laminar gas jet diffusion flames, results from this project (4/1/91 8/22/95) and another NASA study show that flame shape, soot concentration, and radiation heat fluxes are substantially different under microgravity conditions. Our emphasis is on including detailed soot transport models and a detailed solution for radiation heat transfer, and on coupling them with the flame structure calculations. In this paper, we will discuss the following three specific areas: (1) Comparing two existing soot formation models, and identifying possible improvements; (2) A simple yet reasonably accurate approach to calculating total radiative properties and/or fluxes over the spectral range; and (3) Investigating the convergence of iterations between the flame structure solver and the radiation heat transfer solver.

Morphological and semi-quantitative characteristics of diesel soot agglomerates emitted from commercial vehicles and a dynamometer.

PubMed

Luo, Chin-Hsiang; Lee, Whei-May; Liaw, Jiun-Jian

2009-01-01

Diesel soot aggregates emitted from a model dynamometer and 11 on-road vehicles were segregated by a micro-orifice uniform deposit impactor (MOUDI). The elemental contents and morphological parameters of the aggregates were then examined by scanning electron microscopy coupled with an energy dispersive spectrometer (SEM-EDS), and combined with a fractional Brownian motion (fBm) processor. Two mode-size distributions of aggregates collected from diesel vehicles were confirmed. Mean mass concentration of 339 mg/m3 (dC/dlogdp) existed in the dominant mode (180-320 nm). A relatively high proportion of these aggregates appeared in PM1, accentuating the relevance regarding adverse health effects. Furthermore, the fBm processor directly parameterized the SEM images of fractal like aggregates and successfully quantified surface texture to extract Hurst coefficients (H) of the aggregates. For aggregates from vehicles equipped with a universal cylinder number, the H value was independent of engine operational conditions. A small H value existed in emitted aggregates from vehicles with a large number of cylinders. This study found that aggregate fractal dimension related to H was in the range of 1.641-1.775, which is in agreement with values reported by previous TEM-based experiments. According to EDS analysis, carbon content ranged in a high level of 30%-50% by weight for diesel soot aggregates. The presence of Na and Mg elements in these sampled aggregates indicated the likelihood that some engine enhancers composed of biofuel or surfactants were commonly used in on-road vehicles in Taiwan. In particular, the morphological H combined with carbon content detection can be useful for characterizing chain-like or cluster diesel soot aggregates in the atmosphere.

Impacts of Organic Macromolecules, Chlorophyll and Soot on Arctic Sea Ice

NASA Astrophysics Data System (ADS)

Ogunro, O. O.; Wingenter, O. W.; Elliott, S.; Flanner, M.; Dubey, M. K.

2014-12-01

Recent intensification of Arctic amplification can be strongly connected to positive feedback relating black carbon deposition to sea ice surface albedo. In addition to soot deposition on the ice and snow pack, ice algal chlorophyll is likely to compete as an absorber and redistributor of energy. Hence, solar radiation absorption by chlorophyll and some components of organic macromolecules in/under the ice column is currently being examined to determine the level of influence on predicted rate of ice loss. High amounts of organic macromolecules and chlorophyll are produced in global sea ice by the bottom microbial community and also in vertically distributed layers where substantial biological activities take place. Brine channeling in columnar ice can allow for upward flow of nutrients which leads to greater primary production in the presence of moderate light. Modeling of the sea-ice processes in tandem with experiments and field observations promises rapid progress in enhancing Arctic ice predictions. We are designing and conducting global climate model experiments to determine the impact of organic macromolecules and chlorophyll on Arctic sea ice. Influences on brine network permeability and radiation/albedo will be considered in this exercise. Absorption by anthropogenic materials such as soot and black carbon will be compared with that of natural pigments. We will indicate areas of soot and biological absorption dominance in the sense of single scattering, then couple into a full radiation transfer scheme to attribute the various contributions to polar climate change amplification. The work prepares us to study more traditional issues such as chlorophyll warming of the pack periphery and chemical effects of the flow of organics from ice internal communities. The experiments started in the Arctic will broaden to include Antarctic sea ice and shelves. Results from the Arctic simulations will be presented.

Development of a reduced tri-propylene glycol monomethyl ether– n -hexadecane–poly-aromatic hydrocarbon mechanism and its application for soot prediction

DOE PAGES

Park, Seunghyun; Ra, Youngchul; Reitz, Rolf D.; ...

2016-03-01

A reduced chemical kinetic mechanism for Tri-Propylene Glycol Monomethyl Ether (TPGME) has been developed and applied to computational fluid dynamics (CFD) calculations for predicting combustion and soot formation processes. The reduced TPGME mechanism was combined with a reduced n-hexadecane mechanism and a Poly-Aromatic Hydrocarbon (PAH) mechanism to investigate the effect of fuel oxygenation on combustion and soot emissions. The final version of the TPGME-n-hexadecane-PAH mechanism consists of 144 species and 730 reactions and was validated with experiments in shock tubes as well as in a constant volume spray combustion vessel (CVCV) from the Engine Combustion Network (ECN). The effects ofmore » ambient temperature, varying oxygen content in the tested fuels on ignition delay, spray liftoff length and soot formation under diesel-like conditions were analyzed and addressed using multidimensional reacting flow simulations and the reduced mechanism. Here, the results show that the present reduced mechanism gives reliable predictions of the combustion characteristics and soot formation processes. In the CVCV simulations, two important trends were identified. First, increasing the initial temperature in the CVCV shortens the ignition delay and lift-off length, reduces the fuel-air mixing, thereby increasing the soot levels. Secondly, fuel oxygenation introduces more oxygen into the central region of a fuel jet and reduces residence times of fuel rich area in active soot forming regions, thereby reducing soot levels.« less

Development of a reduced tri-propylene glycol monomethyl ether– n -hexadecane–poly-aromatic hydrocarbon mechanism and its application for soot prediction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, Seunghyun; Ra, Youngchul; Reitz, Rolf D.

A reduced chemical kinetic mechanism for Tri-Propylene Glycol Monomethyl Ether (TPGME) has been developed and applied to computational fluid dynamics (CFD) calculations for predicting combustion and soot formation processes. The reduced TPGME mechanism was combined with a reduced n-hexadecane mechanism and a Poly-Aromatic Hydrocarbon (PAH) mechanism to investigate the effect of fuel oxygenation on combustion and soot emissions. The final version of the TPGME-n-hexadecane-PAH mechanism consists of 144 species and 730 reactions and was validated with experiments in shock tubes as well as in a constant volume spray combustion vessel (CVCV) from the Engine Combustion Network (ECN). The effects ofmore » ambient temperature, varying oxygen content in the tested fuels on ignition delay, spray liftoff length and soot formation under diesel-like conditions were analyzed and addressed using multidimensional reacting flow simulations and the reduced mechanism. Here, the results show that the present reduced mechanism gives reliable predictions of the combustion characteristics and soot formation processes. In the CVCV simulations, two important trends were identified. First, increasing the initial temperature in the CVCV shortens the ignition delay and lift-off length, reduces the fuel-air mixing, thereby increasing the soot levels. Secondly, fuel oxygenation introduces more oxygen into the central region of a fuel jet and reduces residence times of fuel rich area in active soot forming regions, thereby reducing soot levels.« less

Fluxes of Soot Carbon to South Atlantic Sediments

EPA Science Inventory

Deep sea sediment samples from the South Atlantic Ocean were analyzed for soot black carbon (BC), total organic carbon (TOC), stable carbon isotope ratios (δ 13C), and polycyclic aromatic hydrocarbons (PAHs). Soot BC was present at low concentrations (0.04–0.17% dry weight), but ...

RELATIONSHIP BETWEEN PCB PLANERITY AND INTERACTIONS WITH SOOT CARBON

EPA Science Inventory

There is increasing interest in the role of soot carbon in the strong partitioning of organic contaminants to sediments. Primary interest has been focused on PAHs which have been shown to be affected by the presence of soot carbon in both their geochemical and bioavailability beh...

T-matrix Study of Scattering and Absorption of Light by Biomass Burning Aerosols

NASA Astrophysics Data System (ADS)

Poudel, Samin

The uncertainty in the measurements of aerosol optical properties has made it difficult to quantify the global impact of aerosols on Earth's climate and limits our ability to predict future climate changes. Morphology, size, volume, shape, fuel type, burning conditions, aging, and changes in chemical composition due to atmospheric processing of soot play a significant part in determining the optical properties of aerosols. The T-matrix method has been successfully used to reproduce experimental results of optical properties of spherical and non-spherical particles. In this work we applied the T-matrix method to extract the refractive index of biomass burning soot (burning pine tree) by reproducing experimentally determined single scattering albedo (SSA), scattering and extinction cross section values obtained by burning pine and collecting aerosols in two different ways: (1) from an outdoor burn drum to burn pine and collect soot in distilled water using an impinger and re-aerosolized the soot after several days to measure extinction and scattering cross sections using cavity ring down spectroscopy and nephelometry and (2) from a tube furnace in the lab to burn pine and the soot was introduced into an indoor smog chamber and soot particles sampled directly into the cavity ring down system and the nephelometer to measure extinction and scattering cross sections. Filter samples were also collected from both types of burning and electron microscopy images were used to obtain morphology and size information to conduct T-Matrix calculations. The experimentally measured optical properties from the impinger samples were reproduced using a refractive index of 1.345 + i0.096 for 300 and 400nm particles, while the results from the tube furnace samples were reproduced using 1.88 + i0.024 for 200 nm particles and 1.47 + i0.047 for 300 nm particles. This suggests that the impinger samples do not represent fresh soot since they are more absorbing and have lower SSA values compared to ours and other similar laboratory and field measurements for fresh soot. Morphology information from images of filter samples was used in the T-matrix calculation using refractive index of 1.88 + i0.024 to reproduce the SSA values for the fresh soot. It is shown that refractive indices used for fresh diesel soot or soot produced from propane 1.76 + i0.57 cannot be applied to biomass burning soot, as it provides a significantly lower SSA values in both cases.

Simulation of low temperature combustion mechanism of different combustion-supporting agents in close-coupled DOC and DPF system.

PubMed

Jiao, Penghao; Li, Zhijun; Li, Qiang; Zhang, Wen; He, Li; Wu, Yue

2018-07-01

In the coupled Diesel Oxidation Catalyst (DOC) and Diesel Particular Filter (DPF) system, soot cannot be completely removed by only using the passive regeneration. And DPF active regeneration is necessary. The research method in this paper is to spray different kinds of combustion-supporting agents to the DOC in the front of the DPF. Therefore, the low temperature combustion mechanism of different kinds of combustion-supporting agents in DOC was studied, in order to grasp the law of combustion in DOC, and the influence of follow-up emission on DPF removal of soot. During the study, CH 4 H 2 mixture and diesel (n-heptane + toluene) were used as combustion-supporting agents respectively. The simplified mechanisms of two kinds of gas mixtures used as the combustion-supporting agents in DPF have been constructed and testified in the paper. In this paper, the combustion and emission conditions of the two combustion-supporting agents were analyzed so as to meet the practical requirements of different working conditions. Copyright © 2017 ISA. Published by Elsevier Ltd. All rights reserved.

Raman Spectroscopy of Single Light-Absorbing Carbonaceous Particles Levitated in Air Using an Annular Laser Beam.

PubMed

Uraoka, Masaru; Maegawa, Keisuke; Ishizaka, Shoji

2017-12-05

A laser trapping technique is a powerful means to investigate the physical and chemical properties of single aerosol particles in a noncontact manner. However, optical trapping of strongly light-absorbing particles such as black carbon or soot is quite difficult because the repulsive force caused by heat is orders of magnitude larger than the attractive force of radiation pressure. In this study, a laser trapping and Raman microspectroscopy system using an annular laser beam was constructed to achieve noncontact levitation of single light-absorbing particles in air. Single acetylene carbon black or candle soot particles were arbitrarily selected with a glass capillary connected to a three-axis oil hydraulic micromanipulator and introduced into a minute space surrounded by a repulsive force at the focal point of an objective lens. Using the developed system, we achieved optical levitation of micrometer-sized carbonaceous particles and observation of their Raman spectra in air. Furthermore, we demonstrated in situ observations of changes in the morphology and chemical composition of optically trapped carbonaceous particles in air, which were induced by heterogeneous oxidation reactions with ozone and hydroxyl radicals.

Fuel-rich catalytic combustion: A fuel processor for high-speed propulsion

NASA Technical Reports Server (NTRS)

Brabbs, Theodore A.; Rollbuhler, R. James; Lezberg, Erwin A.

1990-01-01

Fuel-rich catalytic combustion of Jet-A fuel was studied over the equivalence ratio range 4.7 to 7.8, which yielded combustion temperatures of 1250 to 1060 K. The process was soot-free and the gaseous products were similar to those obtained in the iso-octane study. A carbon atom balance across the catalyst bed calculated for the gaseous products accounted for about 70 to 90 percent of the fuel carbon; the balance was condensed as a liquid in the cold trap. It was shown that 52 to 77 percent of the fuel carbon was C1, C2, and C3 molecules. The viability of using fuel-rich catalytic combustion as a technique for preheating a practical fuel to very high temperatures was demonstrated. Preliminary results from the scaled up version of the catalytic combustor produced a high-temperature fuel containing large amounts of hydrogen and carbon monoxide. The balance of the fuel was completely vaporized and in various stages of pyrolysis and oxidation. Visual observations indicate that there was no soot present.

Photographic combustion characterization of LOX/hydrocarbon type propellants

NASA Technical Reports Server (NTRS)

Judd, D. C.

1979-01-01

Single element injectors and two fuels were tested with the aim of photographically characterizing observed combustion phenomena. The three injectors tested were the O-F-O triplet, the transverse like on like (TLOL), and the rectangular unlike doublet (RUD). The fuels tested were RP-1 and propane. The hot firings were conducted in a specifically constructed chamber fitted with quartz windows for photographically viewing the impingement spray field. All LOX/HC testing demonstrated coking with the RP-1 fuel leaving far more soot than the propane fuel. No fuel freezing or popping was experienced under the test conditions evaluated. Carbon particle emission and combustion light brilliance increased with Pc for both fuels although RP-1 was far more energetic in this respect. The RSS phenomena appear to be present in the high Pc tests as evidenced by striations in the spray pattern and by separate fuel rich and oxidizer rich areas. The RUD element was also tested as a fuel rich gas generator element by switching the propellant circuits. Excessive sooting occurred at this low mixture ratio (0.55), precluding photographic data.

PREPARATION AND TESTING OF CORROSIONAND SPALLATION-RESISTANT COATINGS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hurley, John

2014-11-01

This Energy & Environmental Research Center (EERC) project is designed to determine if plating APMT®, a specific highly oxidation-resistant oxide dispersion-strengthened FeCrAl alloy made by Kanthal, onto nickel-based superalloy turbine parts is a viable method for substantially improving the lifetimes and maximum use temperatures of the parts. The method for joining the APMT plate to the superalloys is called evaporative metal bonding and involves placing a thin foil of zinc (Zn) between the plate and the superalloy, clamping them together, and heating in an atmosphere-controlled furnace. Upon heating, the Zn melts and dissolves the oxide skins of the alloys atmore » the bond line, allowing the two alloys to diffuse into each other. The Zn then diffuses through the alloys and evaporates from their surfaces. Laboratory testing to determine the diffusion rate of Zn through the alloys has been completed. However, an analytical solution does not exist to model the diffusion of zinc through the alloys. For this reason, a finite difference algorithm using MATLAB was developed. It makes use of the hopscotch algorithm. The model allows the user to specify the dimensions of the metal parts, the Zn concentration at the bondline, the mesh size, time step, and Zn diffusivity. The experimentally measured values of diffusivity for Zn in APMT and Rene 80/CM 247LC are approximately 2.7 × 10-12 and 4 × 10-14 m2/s, respectively. While the qualitative behavior of the model appears correct, a comparison of the diffusion predictions with the experimental results from earlier in the project indicates that the expected Zn concentration is significantly higher than that measured experimentally. The difference depends on the assumed initial concentration, which is difficult to quantify exactly under experimental conditions for t = 0. In addition to the diffusion work, the coefficients of thermal expansions were determined for each of the alloys as a function of temperature. This information has been entered into a finite element model using ANSYS so that appropriate force-applying structures can be designed for use in joining structures composed of APMT and the nickel alloys. Finite element modeling has been performed to finalize the fabrication geometry for the corrosion-testing phase. The addition of another bolt increases stress uniformity away from the region where the clamping is applied. It appears that a bolt spacing of approximately 25 mm in each jig is appropriate. This will allow the fabrication of 50-mm-wide sections of joints for the corrosion-testing task. Gasifier sampling activities continue to determine what types of trace contaminants may occur in cleaned syngas that could lead to corrosion or deposition in turbines firing coal syngas. The EERC has several pilot-scale gasifiers that are continually used in a variety of test configurations as determined by the needs of the projects that are funding the tests. We are sampling both noncombusted and combusted syngas produced during some of the pilot-scale gasifier tests. This year sampling was performed of both syngas and combusted syngas while the entrained-flow gasifier (EFG) was firing subbituminous coal from the Antelope Mine in Wyoming. Results of scanning electron microscope analyses of the syngas before combustion showed no submicron particles, only flakes of iron oxide that had likely formed on steel surfaces inside the combustor. As shown in the 2013 annual report, soot was also collected from the syngas when the much-lower-temperature fluid-bed gasifier (FBG) was fired, indicating that the much higher temperature of the EFG prevented soot formation. However, particles collected from the combusted syngas consist almost entirely of submicron soot, and little to no vaporized metals made it past the warm-gas filters and scrubbers in the high-temperature EFG system which could then deposit in a turbine system burning a higher hydrogen syngas. These results are consistent with the analyses of the particulates collected from combusted syngas when the lowertemperature FBG system is used.« less

Characterization of Diesel Soot Aggregates by Scattering and Extinction Methods

NASA Astrophysics Data System (ADS)

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.

Aggregates and Superaggregates of Soot with Four Distinct Fractal Morphologies

NASA Technical Reports Server (NTRS)

Sorensen, C. M.; Kim, W.; Fry, D.; Chakrabarti, A.

2004-01-01

Soot formed in laminar diffusion flames of heavily sooting fuels evolves through four distinct growth stages which give rise to four distinct aggregate fractal morphologies. These results were inferred from large and small angle static light scattering from the flames, microphotography of the flames, and analysis of soot sampled from the flames. The growth stages occur approximately over four successive orders of magnitude in aggregate size. Comparison to computer simulations suggests that these four growth stages involve either diffusion limited cluster aggregation or percolation in either three or two dimensions.

Characterization and Demonstrations of Laser-Induced Incandescence in both Normal and Low-Gravity

NASA Technical Reports Server (NTRS)

VanderWal, Randall L.

1997-01-01

Knowledge of soot volume fraction is important to a wide range of combustion studies in microgravity. Laser-induced incandescence (LII) offers high sensitivity, high temporal and spatial resolution in addition to geometric versatility for real-time determination of soot volume fraction. Implementation of LII into the 2.2 see drop tower at The NASA-Lewis Research Center along with system characterization is described. Absolute soot volume fraction measurements are presented for laminar and turbulent gas-jet flames in microgravity to illustrate the capabilities of LII in microgravity. Comparison between LII radial intensity profiles with soot volume fraction profiles determined through a full-field light extinction technique are also reported validating the accuracy of LII for soot volume fraction measurements in a microgravity environment.

Carbon Nanostructure of Diesel Soot Particles Emitted from 2 and 4 Stroke Marine Engines Burning Different Fuels.

PubMed

Lee, Won-Ju; Park, Seul-Hyun; Jang, Se-Hyun; Kim, Hwajin; Choi, Sung Kuk; Cho, Kwon-Hae; Cho, Ik-Soon; Lee, Sang-Min; Choi, Jae-Hyuk

2018-03-01

Diesel soot particles were sampled from 2-stroke and 4-stroke engines that burned two different fuels (Bunker A and C, respectively), and the effects of the engine and fuel types on the structural characteristics of the soot particle were analyzed. The carbon nanostructures of the sampled particles were characterized using various techniques. The results showed that the soot sample collected from the 4-stroke engine, which burned Bunker C, has a higher degree of order of the carbon nanostructure than the sample collected from the 2-stroke engine, which burned Bunker A. Furthermore, the difference in the exhaust gas temperatures originating from the different engine and fuel types can affect the nanostructure of the soot emitted from marine diesel engines.

A Computational Investigation of Sooting Limits of Spherical Diffusion Flames

NASA Technical Reports Server (NTRS)

Lecoustre, V. R.; Chao, B. H.; Sunderland, P. B.; Urban, D. L.; Stocker, D. P.; Axelbaum, R. L.

2007-01-01

Limiting conditions for soot particle inception in spherical diffusion flames were investigated numerically. The flames were modeled using a one-dimensional, time accurate diffusion flame code with detailed chemistry and transport and an optically thick radiation model. Seventeen normal and inverse flames were considered, covering a wide range of stoichiometric mixture fraction, adiabatic flame temperature, and residence time. These flames were previously observed to reach their sooting limits after 2 s of microgravity. Sooting-limit diffusion flames with residence times longer than 200 ms were found to have temperatures near 1190 K where C/O = 0.6, whereas flames with shorter residence times required increased temperatures. Acetylene was found to be a reasonable surrogate for soot precursor species in these flames, having peak mole fractions of about 0.01.

Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing

PubMed Central

Zhang, Renyi; Khalizov, Alexei F.; Pagels, Joakim; Zhang, Dan; Xue, Huaxin; McMurry, Peter H.

2008-01-01

The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by ≈10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing. PMID:18645179

A multi-probe thermophoretic soot sampling system for high-pressure diffusion flames

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vargas, Alex M.; Gülder, Ömer L.

Optical diagnostics and physical probing of the soot processes in high pressure combustion pose challenges that are not faced in atmospheric flames. One of the preferred methods of studying soot in atmospheric flames is in situ thermophoretic sampling followed by transmission electron microscopy imaging and analysis for soot sizing and morphology. The application of this method of sampling to high pressures has been held back by various operational and mechanical problems. In this work, we describe a rotating disk multi-probe thermophoretic soot sampling system, driven by a microstepping stepper motor, fitted into a high-pressure chamber capable of producing sooting laminarmore » diffusion flames up to 100 atm. Innovative aspects of the sampling system design include an easy and precise control of the sampling time down to 2.6 ms, avoidance of the drawbacks of the pneumatic drivers used in conventional thermophoretic sampling systems, and the capability to collect ten consecutive samples in a single experimental run. Proof of principle experiments were performed using this system in a laminar diffusion flame of methane, and primary soot diameter distributions at various pressures up to 10 atm were determined. High-speed images of the flame during thermophoretic sampling were recorded to assess the influence of probe intrusion on the flow field of the flame.« less

Ambient Observations of the Soot Aging Process during the SHARP Intensive Field Campaign

NASA Astrophysics Data System (ADS)

Reed, C.; Collins, D. R.; Khalizov, A. F.; Zheng, J.; Zhang, R.

2009-12-01

Soot aerosols affect climate both directly through absorption of solar radiation and indirectly by potentially serving as cloud condensation nuclei. Among the sources of uncertainty surrounding the effects of soot aerosol on the environment is the lack of scientific insight into the soot aging process, in which soot particles develop a coating of secondary species such as sulfates, ammonium, nitrate, and organics. Such processes may alter the behavior of soot by modifying particle morphology over time leading to changes in chemical, physical and scattering properties of the aerosol. However, it is often difficult to quantify such processes in the ambient environment due to the complex composition and spatial and temporal variability of the atmospheric aerosol. In order to better understand the effects of the environment on soot particles, it is desirable to study the processes responsible for their transformation in the ambient air without influence from variability in source region and history prior to sampling. To achieve this, the overall soot aging process in the ambient environment was physically isolated utilizing environmental chambers. Chamber measurements were conducted on the Moody Tower at the University of Houston using The Ambient Aerosol Chamber for Evolution Studies (AACES) during the SHARP campaign. AACES is a roughly cubical chamber constructed of a rigid acrylic outer shell, which transmits UV radiation both in the UV-B and UV-A ranges. FEP Teflon lines the inside of the chamber on all sides and the top, while expanded-PTFE (ePTFE) Teflon is used on the bottom of the chamber. The fibrous structure of the ePTFE acts as a barrier to particulates, while allowing gas molecules to move virtually unimpeded from the surrounding air into the chamber, creating an environment inside the chamber that is initially free of particles and continuously mimics the local ambient air. In order to study the effects of the soot aging process, a non-premixed propane flame was used to generate a polydisperse fresh soot aerosol. Then, using a differential mobility analyzer, a monodisperse, uncharged soot aerosol was injected into the environmental chamber. Observations of particle concentration, size, hygroscopicity, effective density, and light extinction and scattering properties were carried out over time using a tandem differential mobility analyzer system, an aerosol particle mass analyzer, a nephelometer and a cavity ringdown spectrometer. Results from preliminary analysis of the data collected during the campaign will be presented.

Elemental carbon and polycyclic aromatic compounds in a 150-year sediment core from Lake Qinghai, Tibetan Plateau, China: influence of regional and local sources and transport pathways.

PubMed

Han, Y M; Wei, C; Bandowe, B A M; Wilcke, W; Cao, J J; Xu, B Q; Gao, S P; Tie, X X; Li, G H; Jin, Z D; An, Z S

2015-04-07

Elemental carbon (EC) and polycyclic aromatic compounds (PACs) are potential proxies for the reconstruction of change in human activities and the origin of air masses in historic times. In this study, the historic deposition of char and soot (the two subtypes of EC) and PACs in a 150-year sediment core from different topographic subbasins of Lake Qinghai on the Qinghai Tibetan Plateau (QTP) were reconstructed. The objective was to explore how the variations in the concentrations of EC and PACs, in the ratios of char to soot and of oxygenated polycyclic aromatic hydrocarbons (OPAHs) to parent PAHs, and in the composition of the PAC mixtures reflect historical changes in climate and human activity and the origin of air masses arriving at the QTP. The deposition fluxes of soot in the different subbasins were similar, averaging 0.18 (range of 0.15-0.25) and 0.16 (0.13-0.23) g m(-2) year(-1), respectively, but they varied for char (averaging 0.11 and 0.22 g m(-2) year(-1), respectively), suggesting ubiquitous atmospheric deposition of soot and local river inputs of char. The different vertical distributions of the char/soot ratios in the different subbasins can be interpreted in terms of the different transport mechanisms of char and soot. An abrupt increase in soot concentrations since 1980 coincides with results from the QTP ice cores that were interpreted to be indicative of soot transport from South Asia. Similar concentration patterns of PAHs with soot and 9,10-anthraquinone/anthracene (9,10-AQ/ANT) ratios all >2.0 suggest regional PAC sources. Increasing PAH/soot ratios and decreasing 9,10-AQ/ANT ratios since the beginning of the 1970s indicate increasing local emissions. The historical trends of these diagnostic ratios indicate an increase in the fossil-fuel contribution since the beginning of the 1970s. The increase of perylene concentrations with increasing core depth and the ratio of perylene to its penta-aromatic isomers indicate that perylene originates mainly from in situ biogenic diagenesis. We demonstrate that the concentrations of EC, char, soot, and PACs in sediments can be used to reconstruct local, regional, and remote sources and transport pathways of pollutants to the QTP.

Bioacessibility of PAHs in fuel soot assessed by an in vitro digestive model: effect of including an absorptive sink.

PubMed

Zhang, Yanyan; Pignatello, Joseph J; Tao, Shu; Xing, Baoshan

2015-03-17

Polycyclic aromatic hydrocarbons (PAHs) associated with soot or black carbon can enter the human digestive tract by unintentional ingestion of soil or other particles. This study investigated the bioaccessibility of 11 PAHs in a composite fuel soot sample using an in vitro digestive model that included silicone sheet as an absorptive sink during the small intestinal digestion stage. The sheet was meant to simulate the passive transfer of PAHs in lumen fluid across the small intestinal epithelium, which was postulated to promote desorption of labile PAHs from the soot by steepening the soot-fluid concentration gradient. We show that the presence of silicone sheet during a 4 h default digestion time significantly increased the apparent bioaccessible fraction (Bapp, %), defined as the sum in the sheet and digestive fluid relative to the total PAH determined. The ability to increase Bapp for most PAHs leveled off above a sheet-to-soot ratio of 2.0 g per 50 mg, indicating that the sheet is an effective absorptive sink and promotes desorption in the mentioned way. Enhancement of Bapp by the sheet correlated positively with the octanol-water partition coefficient (Kow), even though the partition coefficient of PAH between sheet and digestive fluid (which contains bile acid micelles) correlated negatively with Kow. It was hypothesized that PAHs initially in the soot exist in labile and nonlabile states. The fraction of labile PAH still sorbed to the soot residue after digestion, and the maximum possible (limiting) bioaccessibility (Blim) could be estimated by varying the sheet-to-soot ratio. We show conclusively that the increase in bioccessibility due to the presence of the sheet is accounted for by a corresponding decrease in fraction of labile PAH still sorbed to the soot. The Blim ranged from 30.8 to 62.4%, independent of molecular size. The nonlabile fraction of individual PAHs (69.2-37.6% in this case) is therefore large and needs to be taken into account in risk assessment.

Soot and Radiation Measurements in Microgravity Jet Diffusion Flames

NASA Technical Reports Server (NTRS)

Ku, Jerry C.

1996-01-01

The subject of soot formation and radiation heat transfer in microgravity jet diffusion flames is important not only for the understanding of fundamental transport processes involved but also for providing findings relevant to spacecraft fire safety and soot emissions and radiant heat loads of combustors used in air-breathing propulsion systems. Our objectives are to measure and model soot volume fraction, temperature, and radiative heat fluxes in microgravity jet diffusion flames. For this four-year project, we have successfully completed three tasks, which have resulted in new research methodologies and original results. First is the implementation of a thermophoretic soot sampling technique for measuring particle size and aggregate morphology in drop-tower and other reduced gravity experiments. In those laminar flames studied, we found that microgravity soot aggregates typically consist of more primary particles and primary particles are larger in size than those under normal gravity. Comparisons based on data obtained from limited samples show that the soot aggregate's fractal dimension varies within +/- 20% of its typical value of 1.75, with no clear trends between normal and reduced gravity conditions. Second is the development and implementation of a new imaging absorption technique. By properly expanding and spatially-filtering the laser beam to image the flame absorption on a CCD camera and applying numerical smoothing procedures, this technique is capable of measuring instantaneous full-field soot volume fractions. Results from this technique have shown the significant differences in local soot volume fraction, smoking point, and flame shape between normal and reduced gravity flames. We observed that some laminar flames become open-tipped and smoking under microgravity. The third task we completed is the development of a computer program which integrates and couples flame structure, soot formation, and flame radiation analyses together. We found good agreements between model predictions and experimental data for laminar and turbulent flames under both normal and reduced gravity. We have also tested in the laboratory the techniques of rapid-insertion fine-wire thermocouples and emission pyrometry for temperature measurements. These techniques as well as laser Doppler velocimetry and spectral radiative intensity measurement have been proposed to provide valuable data and improve the modeling analyses.

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

NASA Astrophysics Data System (ADS)

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) model can be then substituted for the SNBCK with a reduction in CPU time by a factor of about 20 in the latter case.

Cosmic: Carbon Monoxide And Soot In Microgravity Inverse Combustion

NASA Technical Reports Server (NTRS)

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.

Physicochemical characteristics and toxic effects of ozone-oxidized black carbon particles

NASA Astrophysics Data System (ADS)

Li, Qian; Shang, Jing; Zhu, Tong

2013-12-01

Black carbon (BC) or soot particles formed by combustion are ubiquitous in the atmosphere and have a significant effect on climate and human health. Oxidation can change the physicochemical characteristics of BC, thereby increasing its toxicity. The physicochemical properties of BC and ozone-oxidized BC are investigated in this study through transmission electron microscopy, X-ray photoelectron spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy, ultraviolet-visible spectrophotometry, and electron paramagnetic resonance. The contents of oxygen-containing functional groups, hydrophilicity, water-soluble organic compounds, and free radicals increased after ozone treatment. The redox capacity and cytotoxicity of BC particles were enhanced by ozone oxidation as detected by dithiothreitol (DTT) and 3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyltetrazoliumbromide assays. The redox activities of different BC particles are compared. Particle phase contributed significantly to total redox activity as detected by the DTT assay. Results indicate that BC particles that have undergone aging in the atmosphere may be more toxic and harmful to human health.

COMPARATIVE POTENCY METHOD FOR CANCER RISK ASSESSMENT: APPLICATION TO THE QUANTITATIVE ASSESSMENT OF THE CONTRIBUTION OF COMBUSTION EMISSIONS TO LUNG CANCER RISK

EPA Science Inventory

Combustion sources emit soot particles containing carcinogenic polycyclic organic compounds which are mutagenic in short-term genetic bioassays in microbial and mammalian cells and are tumorigenic in animals. Although soot is considered to be a human carcinogen, soots from differ...

Determination of light extinction efficiency of diesel soot from smoke opacity measurements

NASA Astrophysics Data System (ADS)

Lapuerta, Magín; Martos, Francisco J.; Cárdenas, M. Dolores

2005-10-01

An experimental method for the indirect determination of the light extinction efficiency of the exhaust gas emitted by diesel engines is proposed in this paper, based on the simultaneous measurement of spot opacity and continuous opacity, together with the double modelling of the associated soot concentration. The first model simulates the projection of a differently sized soot particle population enclosed in an exhaust gas sample on the filter of a spot opacimeter. The second one simulates the light extinction caused by the soot particles flowing in the exhaust gas stream in an online continuous opacimeter, on the basis of the Beer-Lambert law. This method is an alternative to other theoretical or semi-empirical complex methods which have proved to be inadequate in the case of soot agglomerates. The application of this method to a set of experimental smoke measurements from a commercial light-duty DI diesel engine typical of vehicle road transportation permitted us to draw conclusions about the effect of different engine conditions on the mean light extinction efficiency of the soot particles flowing in the raw exhaust gas stream.

Soot superaggregates from flaming wildfires and their direct radiative forcing.

PubMed

Chakrabarty, Rajan K; Beres, Nicholas D; Moosmüller, Hans; China, Swarup; Mazzoleni, Claudio; Dubey, Manvendra K; Liu, Li; Mishchenko, Michael I

2014-07-01

Wildfires contribute significantly to global soot emissions, yet their aerosol formation mechanisms and resulting particle properties are poorly understood and parameterized in climate models. The conventional view holds that soot is formed via the cluster-dilute aggregation mechanism in wildfires and emitted as aggregates with fractal dimension Df ≈ 1.8 mobility diameter Dm ≤ 1 μm, and aerodynamic diameter Da ≤ 300 nm. Here we report the ubiquitous presence of soot superaggregates (SAs) in the outflow from a major wildfire in India. SAs are porous, low-density aggregates of cluster-dilute aggregates with characteristic Df ≈ 2.6, Dm > 1 μm, and Da ≤ 300 nm that form via the cluster-dense aggregation mechanism. We present additional observations of soot SAs in wildfire smoke-laden air masses over Northern California, New Mexico, and Mexico City. At 550 nm wavelength, [corrected] we estimate that SAs contribute, per unit optical depth, up to 35% less atmospheric warming than freshly-emitted (D(f) ≈ 1.8) [corrected] aggregates, and ≈90% more warming than the volume-equivalent spherical soot particles simulated in climate models.

Extension of Weighted Sum of Gray Gas Data to Mathematical Simulation of Radiative Heat Transfer in a Boiler with Gas-Soot Media

PubMed Central

Nouri-Borujerdi, Ali; Kazi, Salim Newaz

2014-01-01

In this study an expression for soot absorption coefficient is introduced to extend the weighted-sum-of-gray gases data to the furnace medium containing gas-soot mixture in a utility boiler 150 MWe. Heat transfer and temperature distribution of walls and within the furnace space are predicted by zone method technique. Analyses have been done considering both cases of presence and absence of soot particles at 100% load. To validate the proposed soot absorption coefficient, the expression is coupled with the Taylor and Foster's data as well as Truelove's data for CO2-H2O mixture and the total emissivities are calculated and compared with the Truelove's parameters for 3-term and 4-term gray gases plus two soot absorption coefficients. In addition, some experiments were conducted at 100% and 75% loads to measure furnace exit gas temperature as well as the rate of steam production. The predicted results show good agreement with the measured data at the power plant site. PMID:25143981

Extension of weighted sum of gray gas data to mathematical simulation of radiative heat transfer in a boiler with gas-soot media.

PubMed

Gharehkhani, Samira; Nouri-Borujerdi, Ali; Kazi, Salim Newaz; Yarmand, Hooman

2014-01-01

In this study an expression for soot absorption coefficient is introduced to extend the weighted-sum-of-gray gases data to the furnace medium containing gas-soot mixture in a utility boiler 150 MWe. Heat transfer and temperature distribution of walls and within the furnace space are predicted by zone method technique. Analyses have been done considering both cases of presence and absence of soot particles at 100% load. To validate the proposed soot absorption coefficient, the expression is coupled with the Taylor and Foster's data as well as Truelove's data for CO2-H2O mixture and the total emissivities are calculated and compared with the Truelove's parameters for 3-term and 4-term gray gases plus two soot absorption coefficients. In addition, some experiments were conducted at 100% and 75% loads to measure furnace exit gas temperature as well as the rate of steam production. The predicted results show good agreement with the measured data at the power plant site.

Laser-Induced Incandescence Measurements in Low Gravity

NASA Technical Reports Server (NTRS)

VanderWal, R. L.

1997-01-01

A low-gravity environment offers advantages to investigations concerned with soot growth or flame radiation by eliminating of buoyancy-induced convection. Basic to each type of study is knowledge of spatially resolved soot volume fraction, (f(sub v). Laser-induced incandescence (LII) has emerged as a diagnostic for soot volume fraction determination because it possesses high temporal and spatial resolution, geometric versatility and high sensitivity. Implementation and system characterization of LII in a drop tower that provides 2.2 sec of low-gravity (micro)g) at the NASA Lewis Research Center are described here. Validation of LII for soot volume fraction determination in (micro)g is performed by comparison between soot volume fraction measurements obtained by light extinction [20] and LII in low-gravity for a 50/50 mixture (by volume) of 0 acetylene/nitrogen issuing into quiescent air. Quantitative soot volume fraction measurements within other laminar flames of ethane and propane and a turbulent diffusion flame in (micro)g via LII are also demonstrated. An analysis of LII images of a turbulent acetylene diffusion flame in 1-g and (micro)g is presented.

Soot superaggregates from flaming wildfires and their direct radiative forcing

PubMed Central

Chakrabarty, Rajan K.; Beres, Nicholas D.; Moosmüller, Hans; China, Swarup; Mazzoleni, Claudio; Dubey, Manvendra K.; Liu, Li; Mishchenko, Michael I.

2014-01-01

Wildfires contribute significantly to global soot emissions, yet their aerosol formation mechanisms and resulting particle properties are poorly understood and parameterized in climate models. The conventional view holds that soot is formed via the cluster-dilute aggregation mechanism in wildfires and emitted as aggregates with fractal dimension Df ≈ 1.8 mobility diameter Dm ≤ 1 μm, and aerodynamic diameter Da ≤ 300 nm. Here we report the ubiquitous presence of soot superaggregates (SAs) in the outflow from a major wildfire in India. SAs are porous, low-density aggregates of cluster-dilute aggregates with characteristic Df ≈ 2.6, Dm > 1 μm, and Da ≤ 300 nm that form via the cluster-dense aggregation mechanism. We present additional observations of soot SAs in wildfire smoke-laden air masses over Northern California, New Mexico, and Mexico City. We estimate that SAs contribute, per unit optical depth, up to 35% less atmospheric warming than freshly-emitted (Df ≈ 1.8) aggregates, and ≈90% more warming than the volume-equivalent spherical soot particles simulated in climate models. PMID:24981204

Electron reflection and secondary emission characteristics of sputter-textured pyrolytic graphite surfaces

NASA Technical Reports Server (NTRS)

Wintucky, E. G.; Curren, A. N.; Sovey, J. S.

1981-01-01

Low secondary and reflected primary electron emission from the collector electrode surfaces is important for optimum collector efficiency and hence for high overall efficiency of microwave amplifier tubes used in communication satellites and in military systems. Ion sputter texturing of the surface effectively suppresses electron emission from pyrolytic graphite, which is a promising collector electrode material. Secondary and reflected primary electron emission characteristics of sputter textured pyrolytic graphite surfaces with microstructures of various sizes and densities are presented. The microstructure with the lowest electron emission levels, less than those of soot, consists of a dense array of tall, thin spires.

Effects of laser fluence non-uniformity on ambient-temperature soot measurements using the auto-compensating laser-induced incandescence technique

NASA Astrophysics Data System (ADS)

Liu, Fengshan; Rogak, Steven; Snelling, David R.; Saffaripour, Meghdad; Thomson, Kevin A.; Smallwood, Gregory J.

2016-11-01

Multimode pulsed Nd:YAG lasers are commonly used in auto-compensating laser-induced incandescence (AC-LII) measurements of soot in flames and engine exhaust as well as black carbon in the atmosphere. Such lasers possess a certain degree of fluence non-uniformity across the laser beam even with the use of beam shaping optics. Recent research showed that the measured volume fraction of ambient-temperature soot using AC-LII increases significantly, by about a factor of 5-8, with increasing the laser fluence in the low-fluence regime from a very low fluence to a relatively high fluence of near sublimation. The causes of this so-called soot volume fraction anomaly are currently not understood. The effects of laser fluence non-uniformity on the measured soot volume fraction using AC-LII were investigated. Three sets of LII experiments were conducted in the exhaust of a MiniCAST soot generator under conditions of high elemental carbon using Nd:YAG lasers operated at 1064 nm. The laser beams were shaped and relay imaged to achieve a relatively uniform fluence distribution in the measurement volume. To further homogenize the laser fluence, one set of LII experiments was conducted by using a diffractive optical element. The measured soot volume fractions in all three sets of LII experiments increase strongly with increasing the laser fluence before a peak value is reached and then start to decrease at higher fluences. Numerical calculations were conducted using the experimental laser fluence histograms. Laser fluence non-uniformity is found partially responsible for the soot volume fraction anomaly, but is insufficient to explain the degree of soot volume fraction anomaly observed experimentally. Representing the laser fluence variations by a histogram derived from high-resolution images of the laser beam energy profile gives a more accurate definition of inhomogeneity than a simple averaged linear profile across the laser beam.

Effects of soot by-product from the synthesis of engineered metallofullerene nanomaterials on terrestrial invertebrates.

PubMed

Johnson, David R; Boyd, Robert E; Bednar, Anthony J; Weiss, Charles A; Hull, Matt S; Coleman, Jessica G; Kennedy, Alan J; Banks, Cynthia J; Steevens, Jeffery A

2018-02-23

The synthesis of carbon-based nanomaterials is often inefficient, generating large amounts of soot with metals as waste by-product. Currently, there are no specific regulations for disposal of engineered nanomaterials or the waste by-products resulting from their synthesis, so it is presumed that by-products are disposed of in the same way as the parent (bulk) materials. We studied the terrestrial toxicity of soot from gadolinium metallofullerene nanomanufacturing on earthworms (Eisenia fetida) and isopods (Porcellio scaber). The metallofullerene soot consisted of carbon particle agglomerates in the nanometer and submicrometer ranges (1-100 and 101-999 nm, respectively), with metals used during nanomanufacturing detectable on the particles. Despite high metal concentrations (>100 000 mg/kg) in the soot, only a relatively small amount of metals leached out of a spiked field soil, suggesting only moderate mobility. Seven- and 14-d exposures in field soil demonstrated that the soot was only toxic to earthworms at high concentrations (>10 000 mg/kg); however, earthworms avoided spiked soils at lower concentrations (as low as 500 mg/kg) and at lower soil pH. The presence of soot in food and soil did not cause isopod avoidance. These data demonstrate that metallofullerene soot from nanomanufacturing may only be toxic to earthworms at high concentrations representative of improper disposal or accidental spills. However, our results indicate that terrestrial invertebrates may avoid soils contaminated with soot at sublethal concentrations. Environ Toxicol Chem 2018;9999:1-12. Published 2018 Wiley Periodicals, Inc. on behalf of SETAC. This article is a US government work, and as such, is in the public domain in the United States of America. Published 2018 Wiley Periodicals, Inc. on behalf of SETAC. This article is a US government work, and as such, is in the public domain in the United States of America.

Laminar Soot Processes

NASA Technical Reports Server (NTRS)

2001-01-01

Image of soot (smoke) plume made for the Laminar Soot Processes (LSP) experiment during the Microgravity Sciences Lab-1 mission in 1997. LSP-2 will fly in the STS-107 Research 1 mission in 2002. The principal investigator is Dr. Gerard Faeth of the University of Michigan. LSP uses a small jet burner, similar to a classroom butane lighter, that produces flames up to 60 mm (2.3 in) long. Measurements include color TV cameras and a temperature sensor, and laser images whose darkness indicates the quantity of soot produced in the flame. Glenn Research in Cleveland, OH, manages the project.

AMS+ALS: Kinetic and Product Studies of the Heterogeneous Oxidation of Organic Aerosol at the Advanced Light Source

NASA Astrophysics Data System (ADS)

Kroll, J. H.; Wilson, K. R.; Kessler, S. H.; Browne, E. C.; Nah, T.; Smith, J.; Worsnop, D. R.

2014-12-01

The atmospheric oxidation of condensed-phase organic species can have a major influence on the composition, properties, and impacts of organic aerosol (OA); however the rates and products of such "aging" reactions are poorly constrained. Here we describe a series of laboratory experiments aimed at better understanding one class of aging reactions, the heterogeneous oxidation of OA by gas-phase oxidants. Central to these experiments is the availability of vacuum ultraviolet (VUV) light at the Chemical Dynamics Beamline of the Advanced Light Source at LBNL, which enables the implementation of VUV photoionization aerosol mass spectrometry. This technique allows for the real-time, speciated measurement of OA composition, yielding molecular information that is highly complementary to ensemble data from electron-impact ionization. OA composition is measured with both ionization schemes as a function of oxidant exposure within a flow reactor, providing detailed information on the kinetics and products of heterogeneous oxidation over multiple generations of oxidation. Specific topics investigated include the branching between functionalization and fragmentation of OA components, the formation of secondary organic aerosol from photolytically-generated radical species, and the heterogeneous aging of soot-associated organic species.

Health effects of coal mining and combustion: carcinogens and cofactors.

PubMed Central

Falk, H L; Jurgelski, W

1979-01-01

Some polynuclear aromatics (PNA) have been found to be potent carcinogens for all tissues and organs of experimental animals that have been exposed to them, but different dose levels are needed for these effects. They have been known for decades to cause cancer at the site of application but also at certain sites distant from the area of contact. Although some hydrocarbons are potent and complete carcinogens, the majority of related hydrocarbons was originally found to be inactive. Since they generally appear together, it was important to know more about their interaction, particularly whether they would synergize, or antagonize. The polycyclic hydrocarbons have been studied by subcutaneous injection, where they prove very potent carcinogens. They are also very active on the skin of mice where they produce cancer on prolonged application. Inhalation studies, require larger doses yielded negative results until particulate matter was introduced which facilitated the development of lung tumors. Although iron oxide dust was used initially, other dusts were also capable of enhancing the response of the tissue to benzo(a)pyrene carcinogenesis. This point is of importance, particularly since the inhalation of PNA in situations of air pollution or coal mining involves particulates, although of a different type. Soot is not a homogenous substance and several factors determine its properties. Soots will lose some of the absorbed chemicals during their residence in air, but they retain their PNAs for long periods of time when they reach the soil. The carcinogenicity of PNAs in the adsorbed state may be completely absent, depending on particle size of the soot and availability of eluting capability of the tissues or cells in contact with the soot. Whenever the carcinogenic polynuclear aromatics can be eluted they will be active in producing cancer if their residence is adequate. There seems to be no reason to assume that a large increase in coal combustion in the future will by necessity lead to greater risks of cancer to the coal miners or the general urban dweller, because activities to be started now can take into consideration the requirements necessary for control of air pollution in mines as well as in cities. If new uses of coal will be developed, it will be a completely different situation, and statements about the carcinogenic risk from coal utilization do not apply there. Although some of the same carcinogenic PNAs are involved in the health hazards from those processes, other carcinogens and also cocarcinogens will be present, and the exposed workers will not have the apparent benefits of adsorption of PNAs on soot. PMID:540618

Progression of soot cake layer properties during the systematic regeneration of diesel particulate filters measured with neutron tomography

DOE PAGES

Toops, Todd J.; Pihl, Josh A.; Finney, Charles E. A.; ...

2015-01-16

Although particulate filters (PFs) have been a key component of the emission control system for modern diesel engines, there remain significant questions about the basic regeneration behavior of the filters and how it changes with accumulation of increasing soot layers. This effort describes a systematic deposition and regeneration of particulate matter in 25-mm diameter × 76-mm long wall-flow PFs composed of silicon carbide (SiC) material. The initial soot distributions were analyzed for soot cake thickness using a nondestructive neutron imaging technique. With the PFs intact, it was then possible to sequentially regenerate the samples and reanalyze them, which was performedmore » after nominal 20, 50, and 70 % regenerations. The loaded samples show a relatively uniform distribution of particulate with an increasing soot cake thickness and nearly identical initial density of 70 mg/cm 3. Throughout regeneration, the soot cake thickness initially decreases significantly while the density increases to 80–90 mg/cm 3. After ~50 % regeneration, the soot cake thickness stays relatively constant, but instead, the density decreases as pores open up in the layer (~35 mg/cm 3 at 70 % regeneration). Here, complete regeneration initially occurs at the rear of the PF channels. With this information, a conceptual model of the regeneration is proposed.« less

Progression of soot cake layer properties during the systematic regeneration of diesel particulate filters measured with neutron tomography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Toops, Todd J.; Pihl, Josh A.; Finney, Charles E. A.

Although particulate filters (PFs) have been a key component of the emission control system for modern diesel engines, there remain significant questions about the basic regeneration behavior of the filters and how it changes with accumulation of increasing soot layers. This effort describes a systematic deposition and regeneration of particulate matter in 25-mm diameter × 76-mm long wall-flow PFs composed of silicon carbide (SiC) material. The initial soot distributions were analyzed for soot cake thickness using a nondestructive neutron imaging technique. With the PFs intact, it was then possible to sequentially regenerate the samples and reanalyze them, which was performedmore » after nominal 20, 50, and 70 % regenerations. The loaded samples show a relatively uniform distribution of particulate with an increasing soot cake thickness and nearly identical initial density of 70 mg/cm 3. Throughout regeneration, the soot cake thickness initially decreases significantly while the density increases to 80–90 mg/cm 3. After ~50 % regeneration, the soot cake thickness stays relatively constant, but instead, the density decreases as pores open up in the layer (~35 mg/cm 3 at 70 % regeneration). Here, complete regeneration initially occurs at the rear of the PF channels. With this information, a conceptual model of the regeneration is proposed.« less

On the radiative properties of soot aggregates part 1: Necking and overlapping

NASA Astrophysics Data System (ADS)

Yon, J.; Bescond, A.; Liu, F.

2015-09-01

There is a strong interest in accurately modelling the radiative properties of soot aggregates (also known as black carbon particles) emitted from combustion systems and fires to gain improved understanding of the role of black carbon to global warming. This study conducted a systematic investigation of the effects of overlapping and necking between neighbouring primary particles on the radiative properties of soot aggregates using the discrete dipole approximation. The degrees of overlapping and necking are quantified by the overlapping and necking parameters. Realistic soot aggregates were generated numerically by constructing overlapping and necking to fractal aggregates formed by point-touch primary particles simulated using a diffusion-limited cluster aggregation algorithm. Radiative properties (differential scattering, absorption, total scattering, specific extinction, asymmetry factor and single scattering albedo) were calculated using the experimentally measured soot refractive index over the spectral range of 266-1064 nm for 9 combinations of the overlapping and necking parameters. Overlapping and necking affect significantly the absorption and scattering properties of soot aggregates, especially in the near UV spectrum due to the enhanced multiple scattering effects within an aggregate. By using correctly modified aggregate properties (fractal dimension, prefactor, primary particle radius, and the number of primary particle) and by accounting for the effects of multiple scattering, the simple Rayleigh-Debye-Gans theory for fractal aggregates can reproduce reasonably accurate radiative properties of realistic soot aggregates.

Measurement of the spatially distributed temperature and soot loadings in a laminar diffusion flame using a Cone-Beam Tomography technique

NASA Astrophysics Data System (ADS)

Zhao, Huayong; Williams, Ben; Stone, Richard

2014-01-01

A new low-cost optical diagnostic technique, called Cone Beam Tomographic Three Colour Spectrometry (CBT-TCS), has been developed to measure the planar distributions of temperature, soot particle size, and soot volume fraction in a co-flow axi-symmetric laminar diffusion flame. The image of a flame is recorded by a colour camera, and then by using colour interpolation and applying a cone beam tomography algorithm, a colour map can be reconstructed that corresponds to a diametral plane. Look-up tables calculated using Planck's law and different scattering models are then employed to deduce the temperature, approximate average soot particle size and soot volume fraction in each voxel (volumetric pixel). A sensitivity analysis of the look-up tables shows that the results have a high temperature resolution but a relatively low soot particle size resolution. The assumptions underlying the technique are discussed in detail. Sample data from an ethylene laminar diffusion flame are compared with data in the literature for similar flames. The comparison shows very consistent temperature and soot volume fraction profiles. Further analysis indicates that the difference seen in comparison with published results are within the measurement uncertainties. This methodology is ready to be applied to measure 3D data by capturing multiple flame images from different angles for non-axisymmetric flame.

Darkness after the K-T impact: Effects of soot

NASA Technical Reports Server (NTRS)

Wolbach, Wendy S.; Anders, Edward; Orth, Charles J.

1988-01-01

Dust from the K-T impact apparently settled from the atmosphere in less than 6 months, restoring sunlight to minimum photosynthesis levels in about 4 months. However, the discovery of a global soot component in the boundary clay makes it necessary to reconsider the problem, as soot particles not only are smaller (0.1 vs. about 0.5 micrometer) and thus settle more slowly, but also are better light absorbers (optical depth of 13 mg soot cm(-2) about 1800; and are more resistant to rainout. Still, the darkness cannot have lasted very much longer than 6 months, else no larger animals would have survived. Perhaps the soot coagulated with the rock dust and fell out with it. Evidence on this point may be sought at a relatively undisturbed K-T boundary site, such as Woodside Creek, N.Z. There the boundary clay and lowermost Tertiary strata are finely laminated and show large chemical and isotopic differences on a millimeter scale, apparently representing a detailed time sequence. Researchers studied a 3 m section across the boundary at this site, analyzing the principal forms of carbon (soot, elemental C, kerogen, and carbonate) as well as 33 elements. Correlations among the elements were sought. Apparently soot came early and coagulated with the ejecta, staying with them for the primary fallout and in the next 5 cm, but then parting company, perhaps due to size sorting.

Shapes of soot aerosol particles and implications for their effects on climate

NASA Astrophysics Data System (ADS)

Adachi, Kouji; Chung, Serena H.; Buseck, Peter R.

2010-08-01

Soot aerosol particles (also called light-absorbing, black, or elemental carbon) are major contributors to global warming through their absorption of solar radiation. When embedded in organic matter or sulfate, as is common in polluted areas such as over Mexico City (MC) and other megacities, their optical properties are affected by their shapes and positions within their host particles. However, large uncertainties remain regarding those variables and how they affect warming by soot. Using electron tomography with a transmission electron microscope, three-dimensional (3-D) images of individual soot particles embedded within host particles collected from MC and its surroundings were obtained. From those 3-D images, we calculated the optical properties using a discrete dipole approximation. Many soot particles have open, chainlike shapes even after being surrounded by organic matter and are located in off-center positions within their host materials. Such embedded soot absorbs sunlight less efficiently than if compact and located near the center of its host particle. In the case of our MC samples, their contribution to direct radiative forcing is ˜20% less than if they had a simple core-shell shape, which is the shape assumed in many climate models. This study shows that the shapes and positions of soot within its host particles have an important effect on particle optical properties and should be recognized as potentially important variables when evaluating global climate change.

From fire whirls to blue whirls and combustion with reduced pollution.

PubMed

Xiao, Huahua; Gollner, Michael J; Oran, Elaine S

2016-08-23

Fire whirls are powerful, spinning disasters for people and surroundings when they occur in large urban and wildland fires. Whereas fire whirls have been studied for fire-safety applications, previous research has yet to harness their potential burning efficiency for enhanced combustion. This article presents laboratory studies of fire whirls initiated as pool fires, but where the fuel sits on a water surface, suggesting the idea of exploiting the high efficiency of fire whirls for oil-spill remediation. We show the transition from a pool fire, to a fire whirl, and then to a previously unobserved state, a "blue whirl." A blue whirl is smaller, very stable, and burns completely blue as a hydrocarbon flame, indicating soot-free burning. The combination of fast mixing, intense swirl, and the water-surface boundary creates the conditions leading to nearly soot-free combustion. With the worldwide need to reduce emissions from both wanted and unwanted combustion, discovery of this state points to possible new pathways for reduced-emission combustion and fuel-spill cleanup. Because current methods to generate a stable vortex are difficult, we also propose that the blue whirl may serve as a research platform for fundamental studies of vortices and vortex breakdown in fluid mechanics.

Automated Reflectance Measurement System Designed and Fabricated to Determine the Limits of Atomic Oxygen Treatment of Art Through Contrast Optimization

NASA Technical Reports Server (NTRS)

Sechkar, Edward A.; Stueber, Thomas J.; Rutledge, Sharon K.

2000-01-01

Atomic oxygen generated in ground-based research facilities has been used to not only test erosion of candidate spacecraft materials but as a noncontact technique for removing organic deposits from the surfaces of artwork. NASA has patented the use of atomic oxygen to remove carbon-based soot contamination from fire-damaged artwork. The process of cleaning soot-damaged paintings with atomic oxygen requires exposures for variable lengths of time, dependent on the condition of a painting. Care must be exercised while cleaning to prevent the removal of pigment. The cleaning process must be stopped as soon as visual inspection or surface reflectance measurements indicate that cleaning is complete. Both techniques rely on optical comparisons of known bright locations against known dark locations on the artwork being cleaned. Difficulties arise with these techniques when either a known bright or dark location cannot be determined readily. Furthermore, dark locations will lighten with excessive exposure to atomic oxygen. Therefore, an automated test instrument to quantitatively characterize cleaning progression was designed and developed at the NASA Glenn Research Center at Lewis Field to determine when atomic oxygen cleaning is complete.

PORE STRUCTURE OF SOOT DEPOSITS FROM SEVERAL COMBUSTION SOURCES. (R825303)

EPA Science Inventory

Abstract

Soot was harvested from five combustion sources: a dodecane flame, marine and bus diesel engines, a wood stove, and an oil furnace. The soots ranged from 20% to 90% carbon by weight and molar C/H ratios from 1 to 7, the latter suggesting a highly condensed aro...

Optical characterization of multi-scale morphologically complex heterogeneous media - Application to snow with soot impurities

NASA Astrophysics Data System (ADS)

Dai, Xiaoyu; Haussener, Sophia

2018-02-01

A multi-scale methodology for the radiative transfer analysis of heterogeneous media composed of morphologically-complex components on two distinct scales is presented. The methodology incorporates the exact morphology at the various scales and utilizes volume-averaging approaches with the corresponding effective properties to couple the scales. At the continuum level, the volume-averaged coupled radiative transfer equations are solved utilizing (i) effective radiative transport properties obtained by direct Monte Carlo simulations at the pore level, and (ii) averaged bulk material properties obtained at particle level by Lorenz-Mie theory or discrete dipole approximation calculations. This model is applied to a soot-contaminated snow layer, and is experimentally validated with reflectance measurements of such layers. A quantitative and decoupled understanding of the morphological effect on the radiative transport is achieved, and a significant influence of the dual-scale morphology on the macroscopic optical behavior is observed. Our results show that with a small amount of soot particles, of the order of 1ppb in volume fraction, the reduction in reflectance of a snow layer with large ice grains can reach up to 77% (at a wavelength of 0.3 μm). Soot impurities modeled as compact agglomerates yield 2-3% lower reduction of the reflectance in a thick show layer compared to snow with soot impurities modeled as chain-like agglomerates. Soot impurities modeled as equivalent spherical particles underestimate the reflectance reduction by 2-8%. This study implies that the morphology of the heterogeneities in a media significantly affects the macroscopic optical behavior and, specifically for the soot-contaminated snow, indicates the non-negligible role of soot on the absorption behavior of snow layers. It can be equally used in technical applications for the assessment and optimization of optical performance in multi-scale media.

Influence of fuel injection timing and pressure on in-flame soot particles in an automotive-size diesel engine.

PubMed

Zhang, Renlin; Kook, Sanghoon

2014-07-15

The current understanding of soot particle morphology in diesel engines and their dependency on the fuel injection timing and pressure is limited to those sampled from the exhaust. In this study, a thermophoretic sampling and subsequent transmission electron microscope imaging were applied to the in-flame soot particles inside the cylinder of a working diesel engine for various fuel injection timings and pressures. The results show that the number count of soot particles per image decreases by more than 80% when the injection timing is retarded from -12 to -2 crank angle degrees after the top dead center. The late injection also results in over 90% reduction of the projection area of soot particles on the TEM image and the size of soot aggregates also become smaller. The primary particle size, however, is found to be insensitive to the variations in fuel injection timing. For injection pressure variations, both the size of primary particles and soot aggregates are found to decrease with increasing injection pressure, demonstrating the benefits of high injection velocity and momentum. Detailed analysis shows that the number count of soot particles per image increases with increasing injection pressure up to 130 MPa, primarily due to the increased small particle aggregates that are less than 40 nm in the radius of gyration. The fractal dimension shows an overall decrease with the increasing injection pressure. However, there is a case that the fractal dimension shows an unexpected increase between 100 and 130 MPa injection pressure. It is because the small aggregates with more compact and agglomerated structures outnumber the large aggregates with more stretched chain-like structures.

Suppression of Soot Formation and Shapes of Laminar Jet Diffusion Flames

NASA Technical Reports Server (NTRS)

Xu, F.; Dai, Z.; Faeth, G. M.

2001-01-01

Laminar nonpremixed (diffusion) flames are of interest because they provide model flame systems that are far more tractable for analysis and experiments than practical turbulent flames. In addition, many properties of laminar diffusion flames are directly relevant to turbulent diffusion flames using laminar flamelet concepts. Finally, laminar diffusion flame shapes have been of interest since the classical study of Burke and Schumann because they involve a simple nonintrusive measurement that is convenient for evaluating flame shape predictions. Motivated by these observations, the shapes of round hydrocarbon-fueled laminar jet diffusion flames were considered, emphasizing conditions where effects of buoyancy are small because most practical flames are not buoyant. Earlier studies of shapes of hydrocarbon-fueled nonbuoyant laminar jet diffusion flames considered combustion in still air and have shown that flames at the laminar smoke point are roughly twice as long as corresponding soot-free (blue) flames and have developed simple ways to estimate their shapes. Corresponding studies of hydrocarbon-fueled weakly-buoyant laminar jet diffusion flames in coflowing air have also been reported. These studies were limited to soot-containing flames at laminar smoke point conditions and also developed simple ways to estimate their shapes but the behavior of corresponding soot-free flames has not been addressed. This is unfortunate because ways of selecting flame flow properties to reduce soot concentrations are of great interest; in addition, soot-free flames are fundamentally important because they are much more computationally tractable than corresponding soot-containing flames. Thus, the objectives of the present investigation were to observe the shapes of weakly-buoyant laminar jet diffusion flames at both soot-free and smoke point conditions and to use the results to evaluate simplified flame shape models. The present discussion is brief.

Soot Precursor Material: Spatial Location via Simultaneous LIF-LII Imaging and Characterization via TEM

NASA Technical Reports Server (NTRS)

VanderWal, Randall L.

1996-01-01

The chemical and physical transformation between gaseous fuel pyrolysis products and solid carbonaceous soot represents a critical step in soot formation. In this paper, simultaneous two-dimensional LIF-LII (laser-induced fluorescence - laser-induced incandescence) images identify the spatial location where the earliest identifiable chemical and physical transformation of material towards solid carbonaceous soot occurs along the axial streamline in a normal diffusion flame. The identification of the individual LIF and LII signals is achieved by examining both the excitation wavelength dependence and characteristic temporal decay of each signal. Spatially precise thermophoretic sampling measurements are guided by the LIF-LII images with characterization of the sampled material accomplished via both bright and dark field TEM. Both bright and dark field TEM measurements support the observed changes in photophysical properties which account for conversion of fluorescence to incandescence as fuel pyrolysis products evolve towards solid carbonaceous soot.

Soot volume fraction fields in unsteady axis-symmetric flames by continuous laser extinction technique.

PubMed

Kashif, Muhammad; Bonnety, Jérôme; Guibert, Philippe; Morin, Céline; Legros, Guillaume

2012-12-17

A Laser Extinction Method has been set up to provide two-dimensional soot volume fraction field time history at a tunable frequency up to 70 Hz inside an axis-symmetric diffusion flame experiencing slow unsteady phenomena preserving the symmetry. The use of a continuous wave laser as the light source enables this repetition rate, which is an incremental advance in the laser extinction technique. The technique is shown to allow a fine description of the soot volume fraction field in a flickering flame exhibiting a 12.6 Hz flickering phenomenon. Within this range of repetition rate, the technique and its subsequent post-processing require neither any method for time-domain reconstruction nor any correction for energy intrusion. Possibly complemented by such a reconstruction method, the technique should support further soot volume fraction database in oscillating flames that exhibit characteristic times relevant to the current efforts in the validation of soot processes modeling.

Structure of Soot-Containing Laminar Jet Diffusion Flames

NASA Technical Reports Server (NTRS)

Mortazavi, S.; Sunderland, P. B.; Jurng, J.; Koylu, U. O.; Faeth, G. M.

1993-01-01

The structure and soot properties of nonbuoyant and weakly-buoyant round jet diffusion flames were studied, considering ethylene, propane and acetylene burning in air at pressures of 0.125-2.0 atm. Measurements of flame structure included radiative heat loss fractions, flame shape and temperature distributions in the fuel-lean (overfire) region. These measurements were used to evaluate flame structure predictions based on the conserved-scalar formalism in conjunction with the laminar flamelet concept, finding good agreement betweem predictions and measurements. Soot property measurements included laminar smoke points, soot volume function distributions using laser extinction, and soot structure using thermophoretic sampling and analysis by transmission electron microscopy. Nonbuoyant flames were found to exhibit laminar smoke points like buoyant flames but their properties are very different; in particular, nonbuoyant flames have laminar smoke point flame lengths and residence times that are shorter and longer, respectively, than buoyant flames.

Major wildfires at the Cretaceous-Tertiary boundary

NASA Technical Reports Server (NTRS)

Gilmour, Iain; Wolbach, Wendy S.; Anders, Edward

1989-01-01

K-T boundary (KTB) clays from five sites are enriched in soot and charcoal by factors of 100-1000 over Cretaceous levels, apparently due to a global fire. The soot profile nearly coincides with the Ir profile, implying that the fire was triggered by the impact. Much or all of the fuel was biomass, as indicated by the presence of retene and by the C isotopic composition. The amount of elemental C at the KTB (0.012 g/sq cm) is very large, and requires either that most of the Cretaceous biomass burned down or that the soot yield was higher than in small fires. At undisturbed sites, soot correlates tightly with Ir, As, Sb, and Zn. Apparently soot and Ir-bearing ejecta particles coagulated in the stratosphere and then scavenged additional chalcophiles from the hydrosphere. In view of this coagulation, the K-T fire would only slightly prolong the period of darkness and cold caused by impact ejecta.

Model compound study of the pathways for aromatic hydrocarbon formation in soot.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tomczyk, N. A.; Hunt, J. E.; Winans, R. E.

2002-04-29

To explore the mechanisms for formation of aromatic hydrocarbons as precursors to soot, a model system using combustion of biphenyl in a fuel rich flame is studied. The soots acquired at three different temperatures are solvent extracted and the extract characterized by both GCMS and high resolution mass spectrometry. A description of the NMR results for the whole soots has been published (1). The production of most products could be rationalized from the coupling of biphenyls and subsequent aromatic species and the addition of acetylenes to existing aromatic molecules. Early work by Badger on pyrolysis of hydrocarbons is used inmore » developing these schemes (2). The reaction schemes to produce larger aromatic hydrocarbons will be discussed. Richter and Howard have discussed in detail potential reaction mechanisms in the formation of aromatics as precursors to soot (3).« less

Saving Humanity from Catastrophic Cooling with Geo-Engineering

NASA Astrophysics Data System (ADS)

Haapala, K.; Singer, S. F.

2016-02-01

There are two kinds of ice ages; they are fundamentally different and therefore require different methods of mitigation: (i) Major (Milankovitch-style) glaciations occur on a 100,000-year time-scale and are controlled astronomically. (ii) "Little" ice ages were discovered in ice cores; they have been occurring on an approx. 1000-1500-yr cycle and are likely controlled by the Sun [Ref: Singer & Avery 2007. Unstoppable Global Warming: Every 1500 years]. The current cycle's cooling phase may be imminent - hence there may be urgent need for action. To stop onset of a major (Milankovitch) glaciation 1. Locate a "trigger" - a growing perennial snow/ice field - using satellites 2. Spread soot, to lower the albedo, and use Sun to melt 3. How much soot? How to apply soot? Learn by experimentation To lessen (regional, intermittent) cooling of DOB (Dansgaard-Oeschger-Bond) cycles1. Use greenhouse effect of manmade cirrus (ice particles) [Ref: Singer 1988. Meteorology and Atmospheric Physics 38:228 - 239]2. Inject water droplets (mist) near tropopause 3. Trace dispersion of cirrus cloud by satellite and observe warming at surface 4. How much water; over what area? How often to inject? Learn by experimentation Many scientific questions remain. While certainly interesting and important, there is really no need to delay the crucial and urgent tests of geo-engineering, designed to validate schemes of mitigation. Such proposed tests involve only minor costs and present negligible risks to the environment.

Biological effects of carbon black nanoparticles are changed by surface coating with polycyclic aromatic hydrocarbons.

PubMed

Lindner, Karina; Ströbele, Michael; Schlick, Sandra; Webering, Sina; Jenckel, André; Kopf, Johannes; Danov, Olga; Sewald, Katherina; Buj, Christian; Creutzenberg, Otto; Tillmann, Thomas; Pohlmann, Gerhard; Ernst, Heinrich; Ziemann, Christina; Hüttmann, Gereon; Heine, Holger; Bockhorn, Henning; Hansen, Tanja; König, Peter; Fehrenbach, Heinz

2017-03-21

Carbon black nanoparticles (CBNP) are mainly composed of carbon, with a small amount of other elements (including hydrogen and oxygen). The toxicity of CBNP has been attributed to their large surface area, and through adsorbing intrinsically toxic substances, such as polycyclic aromatic hydrocarbons (PAH). It is not clear whether a PAH surface coating changes the toxicological properties of CBNP by influencing their physicochemical properties, through the specific toxicity of the surface-bound PAH, or by a combination of both. Printex ® 90 (P90) was used as CBNP; the comparators were P90 coated with either benzo[a]pyrene (BaP) or 9-nitroanthracene (9NA), and soot from acetylene combustion that bears various PAHs on the surface (AS-PAH). Oxidative stress and IL-8/KC mRNA expression were determined in A549 and bronchial epithelial cells (16HBE14o-, Calu-3), mouse intrapulmonary airways and tracheal epithelial cells. Overall toxicity was tested in a rat inhalation study according to Organization for Economic Co-operation and Development (OECD) criteria. Effects on cytochrome monooxygenase (Cyp) mRNA expression, cell viability and mucociliary clearance were determined in acute exposure models using explanted murine trachea. All particles had similar primary particle size, shape, hydrodynamic diameter and ζ-potential. All PAH-containing particles had a comparable specific surface area that was approximately one third that of P90. AS-PAH contained a mixture of PAH with expected higher toxicity than BaP or 9NA. PAH-coating reduced some effects of P90 such as IL-8 mRNA expression and oxidative stress in A549 cells, granulocyte influx in the in vivo OECD experiment, and agglomeration of P90 and mucus release in the murine trachea ex vivo. Furthermore, P90-BaP decreased particle transport speed compared to P90 at 10 μg/ml. In contrast, PAH-coating induced IL-8 mRNA expression in bronchial epithelial cell lines, and Cyp mRNA expression and apoptosis in tracheal epithelial cells. In line with the higher toxicity compared to P90-BaP and P90-9NA, AS-PAH had the strongest biological effects both ex vivo and in vivo. Our results demonstrate that the biological effect of CBNP is determined by a combination of specific surface area and surface-bound PAH, and varies in different target cells.

Air quality implications of the Deepwater Horizon oil spill.

PubMed

Middlebrook, Ann M; Murphy, Daniel M; Ahmadov, Ravan; Atlas, Elliot L; Bahreini, Roya; Blake, Donald R; Brioude, Jerome; de Gouw, Joost A; Fehsenfeld, Fred C; Frost, Gregory J; Holloway, John S; Lack, Daniel A; Langridge, Justin M; Lueb, Rich A; McKeen, Stuart A; Meagher, James F; Meinardi, Simone; Neuman, J Andrew; Nowak, John B; Parrish, David D; Peischl, Jeff; Perring, Anne E; Pollack, Ilana B; Roberts, James M; Ryerson, Thomas B; Schwarz, Joshua P; Spackman, J Ryan; Warneke, Carsten; Ravishankara, A R

2012-12-11

During the Deepwater Horizon (DWH) oil spill, a wide range of gas and aerosol species were measured from an aircraft around, downwind, and away from the DWH site. Additional hydrocarbon measurements were made from ships in the vicinity. Aerosol particles of respirable sizes were on occasions a significant air quality issue for populated areas along the Gulf Coast. Yields of organic aerosol particles and emission factors for other atmospheric pollutants were derived for the sources from the spill, recovery, and cleanup efforts. Evaporation and subsequent secondary chemistry produced organic particulate matter with a mass yield of 8 ± 4% of the oil mixture reaching the water surface. Approximately 4% by mass of oil burned on the surface was emitted as soot particles. These yields can be used to estimate the effects on air quality for similar events as well as for this spill at other times without these data. Whereas emission of soot from burning surface oil was large during the episodic burns, the mass flux of secondary organic aerosol to the atmosphere was substantially larger overall. We use a regional air quality model to show that some observed enhancements in organic aerosol concentration along the Gulf Coast were likely due to the DWH spill. In the presence of evaporating hydrocarbons from the oil, NO(x) emissions from the recovery and cleanup operations produced ozone.

Air quality implications of the Deepwater Horizon oil spill

PubMed Central

Middlebrook, Ann M.; Murphy, Daniel M.; Ahmadov, Ravan; Atlas, Elliot L.; Bahreini, Roya; Blake, Donald R.; Brioude, Jerome; de Gouw, Joost A.; Fehsenfeld, Fred C.; Frost, Gregory J.; Holloway, John S.; Lack, Daniel A.; Langridge, Justin M.; Lueb, Rich A.; McKeen, Stuart A.; Meagher, James F.; Meinardi, Simone; Neuman, J. Andrew; Nowak, John B.; Parrish, David D.; Peischl, Jeff; Perring, Anne E.; Pollack, Ilana B.; Roberts, James M.; Ryerson, Thomas B.; Schwarz, Joshua P.; Spackman, J. Ryan; Warneke, Carsten; Ravishankara, A. R.

2012-01-01

During the Deepwater Horizon (DWH) oil spill, a wide range of gas and aerosol species were measured from an aircraft around, downwind, and away from the DWH site. Additional hydrocarbon measurements were made from ships in the vicinity. Aerosol particles of respirable sizes were on occasions a significant air quality issue for populated areas along the Gulf Coast. Yields of organic aerosol particles and emission factors for other atmospheric pollutants were derived for the sources from the spill, recovery, and cleanup efforts. Evaporation and subsequent secondary chemistry produced organic particulate matter with a mass yield of 8 ± 4% of the oil mixture reaching the water surface. Approximately 4% by mass of oil burned on the surface was emitted as soot particles. These yields can be used to estimate the effects on air quality for similar events as well as for this spill at other times without these data. Whereas emission of soot from burning surface oil was large during the episodic burns, the mass flux of secondary organic aerosol to the atmosphere was substantially larger overall. We use a regional air quality model to show that some observed enhancements in organic aerosol concentration along the Gulf Coast were likely due to the DWH spill. In the presence of evaporating hydrocarbons from the oil, NOx emissions from the recovery and cleanup operations produced ozone. PMID:22205764

Adhesion of Mineral and Soot Aerosols can Strongly Affect their Scattering and Absorption Properties

NASA Technical Reports Server (NTRS)

Mishchenko, Michael I.; Dlugach, Jana M.

2012-01-01

We use the numerically exact superposition T-matrix method to compute the optical cross sections and the Stokes scattering matrix for polydisperse mineral aerosols (modeled as homogeneous spheres) covered with a large number of much smaller soot particles. These results are compared with the Lorenz-Mie results for a uniform external mixture of mineral and soot aerosols. We show that the effect of soot particles adhering to large mineral particles can be to change the extinction and scattering cross sections and the asymmetry parameter quite substantially. The effect on the phase function and degree of linear polarization can be equally significant.

Flame Structure and Scalar Properties in Microgravity Laminar Fires

NASA Technical Reports Server (NTRS)

Feikema, D. A.; Lim, J.; Sivathanu, Y.

2006-01-01

Recent results from microgravity combustion experiments conducted in the Zero Gravity Facility (ZGF) 5.18 second drop tower are reported. Emission mid-infrared spectroscopy measurements have been completed to quantitatively determine the flame temperature, water and carbon dioxide vapor concentrations, radiative emissive power, and soot concentrations in a microgravity laminar ethylene/air flame. The ethylene/air laminar flame conditions are similar to previously reported experiments including the Flight Project, Laminar Soot Processes (LSP). Soot concentrations and gas temperatures are in reasonable agreement with similar results available in the literature. However, soot concentrations and flame structure dramatically change in long duration microgravity laminar diffusion flames as demonstrated in this paper.