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NASA NTRS2002

Combustion Synthesis of Fullerenes and Fullerenic Nanostructures In Microgravity

The objectives of the proposed research were to determine the effects of gravity on fullerenes formation in flames and, based on the observed effects, to develop fundamental understanding of fullerenes formation and to identify engineering principles for fullerenes production. The research method consisted of the operation of laminar diffusion flames under normal- and reduced-gravity conditions, and the collection from the flames and subsequent analysis of condensables including any fullerenes present, using coupled high performance liquid chromatography/mass spectrometry and high resolution transmission electron microscopy. The focus included fullerene molecules C60 and C70 and fullerenic nanostructures including tubes, spherules and other shapes. The normal-gravity experiments were performed at MIT and complementary reduced-gravity experiments were to have been contributed by NASA. The independent variables of interest are gravity, fuel type, fuel/oxygen ratio, pressure, gas velocity at burner, diluent type and concentration. Given the large number of variables and the absence of data on either fullerene formation in diffusion flames or gravitational effects on fullerene formation in diffusion or premixed flames, the first part of the work was exploratory while the later part involved detailed study of the most interesting mechanisms. Samples of condensable material from laminar low pressure benzene/argon/oxygen diffusion flames were collected and analyzed by high-performance liquid chromatography to determine the yields of fullerenes, and by high-resolution transmission electron microscopy (HRTEM) to characterize the fullerenic material, i.e., curved-layer nanostructures, on and within the soot particles. The highest concentration of fullerenes was always detected just above the visible stoichiometric surface of a flame. The percentage of fullerenes in the condensable material increases with decreasing pressure. The overall highest amount of fullerenes was found for a surprisingly high dilution fuel with argon. The maximum flame temperature seems to be of minor importance in fullerene formation. The HRTEM analysis of the soot showed an increase of the curvature of the carbon layers, and hence increased fullerenic character. After this maximum, the curvature decreases. In addition to the soot, the samples included fullerenic nanostructures, such as tubes and spheroids including highly-ordered multilayered or onion-like structures. The soot itself shows highly ordered regions that appear to have been cells of ongoing fullerenic nanostructure formation.

Howard, Jack B.↗

NASA NTRS1998

Stratospheric Aerosol Measurements

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses implicating manmade fluorocarbons as cause of the --'ozone hole'; (5) The current soot loading is too small to be of environmental (radiative and chemical) consequence. However, the fractal nature of soot distinguishes it aerodynamically and radiatively from sulfuric acid droplets such that its stratospheric residence time is longer, mainly because of vertical transport against gravity due to gravito-photophoretic forces. Thus it may accumulate and become of environmental concern in the future.

Pueschel, Rudolf, F.↗

NASA NTRS2001

Flame Shapes of Nonbuoyant Laminar Jet Diffusion Flames

The shapes (flame-sheet and luminous-flame boundaries) of steady nonbuoyant round hydrocarbon-fueled laminar-jet diffusion flames in still and coflowing air were studied both experimentally and theoretically. Flame-sheet shapes were measured from photographs using a CH optical filter to distinguish flame-sheet boundaries in the presence of blue CO2 and OH emissions and yellow continuum radiation from soot. Present experimental conditions included acetylene-, methane-, propane-, and ethylene-fueled flames having initial reactant temperatures of 300 K, ambient pressures of 4-50 kPa, jet exit Reynolds number of 3-54, initial air/fuel velocity ratios of 0-9 and luminous flame lengths of 5-55 mm; earlier measurements for propylene- and 1,3-butadiene-fueled flames for similar conditions were considered as well. Nonbuoyant flames in still air were observed at micro-gravity conditions; essentially nonbuoyant flames in coflowing air were observed at small pressures to control effects of buoyancy. Predictions of luminous flame boundaries from soot luminosity were limited to laminar smokepoint conditions, whereas predictions of flame-sheet boundaries ranged from soot-free to smokepoint conditions. Flame-shape predictions were based on simplified analyses using the boundary layer approximations along with empirical parameters to distinguish flame-sheet and luminous flame (at the laminar smoke point) boundaries. The comparison between measurements and predictions was remarkably good and showed that both flame-sheet and luminous-flame lengths are primarily controlled by fuel flow rates with lengths in coflowing air approaching 2/3 lengths in still air as coflowing air velocities are increased. Finally, luminous flame lengths at laminar smoke-point conditions were roughly twice as long as flame-sheet lengths at comparable conditions due to the presence of luminous soot particles in the fuel-lean region of the flames.

Xu, F.↗

NASA NTRS2000

Smoke-Point Properties of Nonbuoyant Round Laminar Jet Diffusion Flames

The laminar smoke-point properties of non-buoyant round laminar jet diffusion flames were studied emphasizing results from long-duration (100-230 s) experiments at microgravity carried out in orbit aboard the space shuttle Columbia. Experimental conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K, pressures of 35-130 kPa, jet exit diameters of 1.6 and 2.7 mm, jet exit velocities of 170-690 mm/s, jet exit Reynolds numbers of 46-172, characteristic flame residence times of 40-302 ms, and luminous flame lengths of 15-63 mm. Contrary to the normal-gravity laminar smoke point, in microgravity the onset of laminar smoke-point conditions involved two flame configurations: closed-tip flames with soot emissions along the flame axis and open-tip flames with soot emissions from an annular ring about the flame axis. Open-tip flames were observed at large characteristic flame residence times with the onset of soot emissions associated with radiative quenching near the flame tip: nevertheless, unified correlations of laminar smoke-point properties were obtained that included both flame configurations. Flame lengths at laminar smoke-point conditions were well correlated in terms of a corrected fuel flow rate suggested by a simplified analysis of flame shape. The present steady and nonbuoyant flames emitted soot more readily than non-buoyant flames in earlier tests using ground-based microgravity facilities and than buoyant flames at normal gravity, as a result of reduced effects of unsteadiness, flame disturbances, and buoyant motion. For example, present measurements of laminar smokepoint flame lengths at comparable conditions were up to 2.3 times shorter than ground-based microgravity measurements and up to 6.4 times shorter than buoyant flame measurements. Finally, present laminar smoke-point flame lengths were roughly inversely proportional to pressure to a degree that is a somewhat smaller than observed during earlier tests both at microgravity (using ground-based facilities) and at normal gravity,

Urban, D. L.↗

NASA NTRS2003

Preliminary Assessment Of The Burning Dynamics Of Jp8 Droplets In Microgravity

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.

Bae, J. H.↗

NASA NTRS2000

Flame Design: A Novel Approach Developed to Produce Clean, Efficient Diffusion Flames

Soot formation and flame extinction are vital concerns in the combustion of fossil fuels. In particular, soot is responsible for pollutant emissions, and extinction can cause inefficient or unstable burning. Normal-gravity experiments have demonstrated that flames can be designed to improve both characteristics by redirecting some or all of the nitrogen from the oxidizer into the fuel. Such nitrogen exchange can produce permanently blue flames, which are soot free under all possible flame conditions. Furthermore, this approach can lead to stronger, extinction-resistant flames. Past investigations of nitrogen exchange were unable to identify the physical mechanisms responsible for its benefits because these mechanisms cannot be isolated when normal-gravity flames are studied. In contrast, the Diffusion Flame Extinction and Soot Inception (DESI) experiment considers spherical flames, where nearly perfect spherical symmetry affords new levels of control. Because of buoyancy, spherical flames cannot be created in Earth s gravity. DESI was conceived by principal investigator Professor R.L. Axelbaum of Washington University in St. Louis. Tests to date have utilized the 2.2-Second Drop Tower at the NASA Glenn Research Center at Lewis Field. The experiment is slated for testing aboard the International Space Station in a few years. Two mechanisms have been proposed to explain the connection between nitrogen exchange and permanently blue flames. These are the structure (chemical effects) and hydrodynamics (flow direction and speed). In normal-gravity flames, the structure and hydrodynamics are coupled, since nitrogen exchange simultaneously modifies both. Spherical microgravity flames, on the other hand, allow independent control of these factors. Specifically, structure can be modified via nitrogen exchange, and flow direction can be reversed by swapping the ambient and burner-feed gases. In DESI, these variations can be accomplished without changing the theoretical flame temperature.

Axelbaum, Richard L.↗

NASA NTRS2006

Flame Structure and Scalar Properties in Microgravity Laminar Fires

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.

Feikema, D. A.↗

NASA NTRS2007

Flame Radiation, Structure, and Scalar Properties in Microgravity Laminar Fires

Results from microgravity combustion experiments conducted in the Zero Gravity Research Facility (ZGF) 5.18 second drop facility are reported. The results quantify flame radiation, structure, and scalar properties during the early phase of a microgravity fire. 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 microgravity laminar methane/air, ethylene/nitrogen/air and ethylene/air jet flames. The measured peak mole fractions for water vapor and carbon dioxide are found to be in agreement with state relationship predictions for hydrocarbon/air combustion. The ethylene/air laminar flame conditions are similar to previously reported results including those from 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 report.

Feikema, Douglas↗

NASA NTRS2013

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

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

Underwood, Lauren↗

NASA NTRS2016

Climate and Fuel Controls on North American Paleofires: Smoldering to Flaming in the Late-Glacial-Holocene Transition

Smoldering and flaming fires, which emit different proportions of organic (OC) and black carbon (BC, in the form of char and soot), have long been recognized in modern wildfire observations but never in a paleo-record, and little is known about their interactions with climate. Here we show that in the late glacial-early Holocene transition period, when the climate was moist, relatively high quantities of char were deposited in Linsley Pond, Connecticut, USA while soot was more abundant during the warmer and drier early Holocene interval. The highest soot mass accumulation rates (MARs) occurred at the beginning of the Holocene as fuel availability increased through the climatic transition when boreal forests were locally extirpated. These variations with time are related to the different formation pathways of char and soot, which are governed by combustion efficiency. This study provides an approach for differentiating smoldering from flaming combustion in paleo-wildfire reconstructions. Our results suggest that climate and fuel loads control the occurrence of different wildfire types and precipitation may play a key role.

Han, Y. M.↗

DOE OSTI2023

n-Propylbenzene Droplet Combustion: Experiments and Numerical Modeling

n-Propylbenzene (PB, C9H12, 432K boiling point) is important as a constituent in surrogates for some transportation fuels but little is understood about its droplet burning characteristics. We present an experimental and numerical study of a fuel droplet burning under conditions where the sole means of gas transport is fuel evaporation at the droplet surface thereby creating a one-dimensional gas transport that is amenable to detailed numerical modeling. The one-dimensional gas transport that results is amenable to detailed numerical modeling. Initial droplet diameters (Do) ranged from 0.3 mm to about 5 mm to better understand the mechanisms that control burning over such a wide range of Do. For Do < 1 mm droplets were burned while anchored to 14 m SiC fibers within a sealed container in free-fall during which time the droplets were ignited by spark discharge and the burning process recorded by video cameras. Larger and free-floating droplets were studied in the spaced-based platform of the orbiting International Space Station for Do > 1.0 mm which provided unlimited times for experimental observation. Measurements of droplet, flame and soot shell diameters were made and are discussed in the presentation. The experimental results showed formation of optically thick soot clouds developing during burning that required a robust image analysis algorithm to enable measurement of droplet diameter. The measured droplet diameters were well predicted by a numerical model that included soot formation, a PB kinetic mechanism comprising 576 species and 27369 reactions, unsteady gas and liquid transport, variable properties and radiative transport. Flame diameters showed more variability compared to the simulations, depending on how the flame was defined (peak gas temperature and OH concentration). Droplets burned slower as Do was increased and the PB sooting propensity increased with Do. Flame extinction was observed for Do > 3.3 mm indicating a strong effect of radiation as Do was increased compared to the smaller droplet diameters examined where extinction was not experimentally observed. For the largest droplets examined the possibility that the observed extinction is indicative of a transition to cool flame burning is still under investigation.

Guo, Songtao↗

DOE OSTI2020

Zonal-Based Emission Source Term Model for Predicting Particulate Emission Factors in Wildfire Simulations

A physics/chemistry-based numerical model for predicting the emission of fine particles from wildfires is proposed. This model implements the fundamental mechanisms of soot formation in a combustion environment: soot nucleation, surface growth, agglomeration, oxidation, and particle fragmentation. These mechanisms occur on a scale too fine for the discretization of most wildfire models, which need to simulate landscape-scale dynamics. As a result this model implements a zonal approach, where the computed soot particle distribution is partitioned into process zones within a single resolved grid cell. These process zones include: an inception zone (for nucleation), a heating zone (for coagulation, surface growth, and fragmentation), a reaction zone (for oxidation), and a quenched zone (for atmospheric processes). Governing mechanisms are applied to the appropriate zones to predict total particle growth and emission. Additionally, the proposed model is implemented into HIGRAD/FIRETEC, a physics-based wildfire simulation code which couples interactions between fire, fuels, atmosphere, and topography on a landscape scale. Fire simulations among grasslands and conifer forests are performed and compared against experimental data for emission factors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Into the net zero emissions and climate change control: From solid carbon waste to effective solar convertors

Here, in this work, we demonstrate the potential for solar-to-heat conversion of carbon byproducts and their outstanding effects to reduce anthropogenic emissions. Those carbon byproducts are soots (biomass, evaporated carbon, etc.) as well as morphed graphenes. Our results cover optical characterization to demonstrate their suitability as heat capacitors and solar-to-heat convertors. Our raw materials are sustainable and currently considered environmental pollutants that require true attention to minimize global warming effects. Fortunately, they are ideal candidates to reduce the carbon footprints and can contribute towards a true net-zero environmental transition. We explore and demonstrate that soots are among the most competitive materials to transform solar energy into heat due to their absorption capacity, and durability. These materials are more competitive than commercial products and other known solar convertors demonstrating the superior thermosolar benefits. The best candidate is biomass with solar absorptivity, light emission, and cost reduction of 96, 85% and 15-fold, respectively, when compare to commercial products. Biomass and soot have comparable or better solar conversion characteristics, and sustainability than pristine carbon nanostructures and they are up to 3 orders of magnitude cheaper.

14 SOLAR ENERGY↗

DOE OSTI2023

Limitations of cetane number to predict transient combustion phenomena in high-pressure fuel sprays

Fundamental understanding of in-cylinder processes in diesel engines is important to screen emerging biofuels and advanced combustion modes that can reduce greenhouse gas emissions and regulated pollutants including soot. In this study, the role of fuel properties on spray development and combustion is investigated by systematically isolating chemical and thermophysical effects. Three different fuels are considered, two with similar chemical properties and two with similar thermophysical properties with one fuel common to both groups. Experiments are performed in a constant-pressure flow chamber de-signed to provide stable test conditions and facilitate acquisition of at least 150 injections in quick succession for each fuel under reacting conditions at high-pressure, high-temperature ambient conditions using a modified conventional diesel engine injector. Further, high speed optical diagnostics including rainbow schlieren deflectometry, OH* chemiluminescence, and a two-color pyrometry system are employed to simultaneously image the transient spray and reacting jets. Image analysis is performed to determine liquid length, vapor penetration length, timing and location of first stage and main ignition events, lift-off location, total soot mass, and more. Results show that fuels with similar chemical properties or cetane number (CN) exhibit similar delay times for first stage and main ignition events as may be expected, but very different liquid length, first stage and main ignition locations, lift-off length, apparent turbulent flame speed, and soot formation. As such, the ability to characterize candidate biofuels with CN or other parameters derived from simple flame configurations is called into question. In this study, thermo-physical properties controlling the liquid length are identified as the main contributing factor for the observed differences.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2020

Identification of engine oil-derived ash nanoparticles and ash formation process for a gasoline direct-injection engine

Engine oil-derived ash particles emitted from internal combustion (IC) engines are unwanted by-products, after oil is involved in in-cylinder combustion process. Since they typically come out together with particulate emissions, no detail has been reported about their early-stage particles other than agglomerated particles loaded on aftertreatment catalysts and filters. To better understand ash formation process during the combustion process, here differently formulated engine oils were dosed into a fuel system of a gasoline direct injection (GDI) engine that produces low soot mass emissions at normal operating conditions to increase the chances to find stand-alone ash particles separated from soot aggregates in the sub-20-nm size range. In addition to them, ash/soot aggregates in the larger size range were examined using scanning transmission electron microscopy (STEM)-X-ray electron dispersive spectroscopy (XEDS) to present elemental information at different sizes of particles from various oil formulations. The STEM-XEDS results showed that regardless of formulated oil type and particle size, Ca, P and C were always contained, while Zn was occasionally found on relatively large particles, suggesting that these elements get together from an early stage of particle formation. The S, Ca and P K-edge X-ray absorption near edge structure (XANES) analyses were performed for bulk soot containing raw ash. The linear combination approach & cross-checking among XANES results proposed that Ca 5 (OH)(PO 4 ) 2 , Ca 3 (PO 4 ) 2 and Zn 3 (PO 4 ) 2 are potentially major chemical compounds in raw ash particles, when combined with the STEM-XEDS results. Despite many reports that CaSO 4 is a major ash chemical when ash found in DPF/GFP systems was examined, it was observed to be rarely present in raw ashes using the S K-edge XANES analysis, suggesting ash transformation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

PeleMP: The Multiphysics Solver for the Combustion Pele Adaptive Mesh Refinement Code Suite

Combustion encompasses multiscale, multiphase reacting flow physics spanning a wide range of scales from the molecular scales, where chemical reactions occur, to the device scales, where the turbulent flow is affected by the geometry of the combustor. This scale disparity and the limited measurement capabilities from experiments make modeling combustion a significant challenge. Recent advancements in high-performance computing (HPC), particularly with the Department of Energy's Exascale Computing Project (ECP), have enabled high-fidelity simulations of practical applications to be performed. The major physics submodels, including chemical reactions, turbulence, sprays, soot, and thermal radiation, exhibit distinctive computational characteristics that need to be examined separately to ensure efficient utilization of computational resources. This paper presents the multiphysics solver for the Pele code suite, called PeleMP, which consists of models for spray, soot, and thermal radiation. Here, the mathematical and algorithmic aspects of the model implementations are described in detail as well as the verification process. The computational performance of these models is benchmarked on multiple supercomputers, including Frontier, an exascale machine. Results are presented from production simulations of a turbulent sooting ethylene flame and a bluff-body swirl stabilized spray flame with sustainable aviation fuels to demonstrate the capability of the Pele codes for modeling practical combustion problems with multiphysics. This work is an important step toward the exascale computing era for high-fidelity combustion simulations providing physical insights and data for predictive modeling of real-world devices.

42 ENGINEERING↗

NASA NTRS2014

Optics of Water Cloud Droplets Mixed with Black-Carbon Aerosols

We use the recently extended superposition T-matrix method to calculate scattering and absorption properties of micrometer-sized water droplets contaminated by black carbon. Our numerically exact results reveal that, depending on the mode of soot-water mixing, the soot specific absorption can vary by a factor exceeding 6.5. The specific absorption is maximized when the soot material is quasi-uniformly distributed throughout the droplet interior in the form of numerous small monomers. The range of mixing scenarios captured by our computations implies a wide range of remote sensing and radiation budget implications of the presence of black carbon in liquid-water clouds. We show that the popular Maxwell-Garnett effective-medium approximation can be used to calculate the optical cross sections, single-scattering albedo, and asymmetry parameter for the quasi-uniform mixing scenario, but is likely to fail in application to other mixing scenarios and in computations of the elements of the scattering matrix.

soot↗

NASA NTRSDate not supplied

Surrogate Fuel Chemistry from ReaxFF Molecular Dynamics

Reactive molecular dynamics with ReaxFF simulations are used to study the chemistry of four component jet fuel mixtures of n-dodecane, iso-octane, n-propylbenzene, and mesitylene. ReaxFF does not require knowledge of the chemistry a priori providing insight into reactions otherwise not seen in established chemical kinetic mechanisms. The results show that a difference in the local chemical environment can change the fuel decomposition pathways across the surrogate mixtures where the same fuel species are used. These simulations highlight the need to consider cross-chemical interactions in chemical kinetic mechanism development and the importance of resonance stabilized polyaromatic hydrocarbon reactions for soot growth and formation. A method for predicting the threshold sooting index from the carbon species formed at the end of the simulations is established. The results of the simulations are consistent with measurements of the threshold sooting index with the predicted values within 20% of the measured data

Surrogate Fuels↗