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At least 19 records

Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires

The effects of biomass burning aerosols (BBA) on radiative forcing and cloud formation depend on chemical composition and the internal structures of individual particles within smoke plumes. To improve our understanding of the chemical and physical properties of BBA emitted at different times of the day and their evolution during atmospheric aging, we conducted a study as a part of the Fire Influence on Regional to Global Environments and Air Quality field campaign. Particle samples were collected onboard a research aircraft from smoke plumes from a wildfire in eastern Oregon during late afternoon and nighttime flights on August 28, 2019. A time-resolved aerosol collector was used to collect samples on substrates for offline spectromicroscopic imaging to investigate the single-particle characteristics of BBA particles. Approximately 20,400 individual particles from 10 selected samples were analyzed using computer-controlled scanning electron microscopy coupled with energy-dispersive X-ray microanalysis, revealing their elemental composition, morphology, and viscosity. Elemental microanalysis indicated that aged potassium is likely found in the form of K 2 SO 4 , KNO 3 , and possible K-organic salts. Further chemical speciation and carbon bonding mapping within individual particles were conducted using synchrotron-based scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure (NEXAFS) spectroscopy. Real-time, water-soluble light absorption measurements were acquired using a particle-into-liquid sampler instrument coupled to a liquid waveguide capillary cell and total organic analyzer. In the late afternoon samples, 65% of the total particle number population consisted entirely of organic components, compared to 46% in the nighttime particles. These differences were attributed to discrepancies in composition at the time of emission and to the daytime condensation and accumulation of photochemically formed secondary organic material on existing BBA particles, a process that halts at night. Microscopy images indicated that particle viscosity was lower in the nighttime particles (<10 1 Pa·s), likely due to increased relative humidity and a higher contribution from hygroscopic inorganic components. The chemical heterogeneity of individual particles was quantified using STXM-derived mixing state parameters. The nature of carbon bonding within individual particles was inferred from the extent of carbon sp 2 hybridization derived from NEXAFS spectra. Average percentages of sp 2 hybridization range between 40% and 60%, with no noticeable differences between late afternoon and nighttime flights. These findings were compared with the online optical properties of both late afternoon and nighttime smoke plumes, providing valuable insights into the complex relationship between chemical composition and optical properties of BBA particles at different times of the day.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Seasonal Trend of Single Scattering Albedo in Southern African Biomass-burning Particles: Implications for Satellite Products and Estimates of Emissions for the World's Largest Biomass-burning Source

As a representative site of the southern African biomass-burning region, sun-sky data from the 15 year Aerosol Robotic Network (AERONET) deployment at Mongu, Zambia, was analyzed. For the biomass-burning season months (July-November), we investigate seasonal trends in aerosol single scattering albedo (SSA), aerosol size distributions, and refractive indices from almucantar sky scan retrievals. The monthly mean single scattering albedo at 440 nm in Mongu was found to increase significantly from approx.. 0.84 in July to approx. 0.93 in November (from 0.78 to 0.90 at 675 nm in these same months). There was no significant change in particle size, in either the dominant accumulation or secondary coarse modes during these months, nor any significant trend in the Angstrom exponent (440-870 nm; r(exp 2) = 0.02). A significant downward seasonal trend in imaginary refractive index (r(exp 2) = 0.43) suggests a trend of decreasing black carbon content in the aerosol composition as the burning season progresses. Similarly, burning season SSA retrievals for the Etosha Pan, Namibia AERONET site also show very similar increasing single scattering albedo values and decreasing imaginary refractive index as the season progresses. Furthermore, retrievals of SSA at 388 nm from the Ozone Monitoring Instrument satellite sensor show similar seasonal trends as observed by AERONET and suggest that this seasonal shift is widespread throughout much of southern Africa. A seasonal shift in the satellite retrieval bias of aerosol optical depth from the Moderate Resolution Imaging Spectroradiometer collection 5 dark target algorithm is consistent with this seasonal SSA trend since the algorithm assumes a constant value of SSA. Multi-angle Imaging Spectroradiometer, however, appears less sensitive to the absorption-induced bias.

aerosol absorption↗

Burning of particles undergoing stripping breakup

A simple model for condensed-phase particle burning has been presented. Particles are assumed to start burning in quiescent air. Particles are then accelerated, adding convective effects. Convective effect due to the relative motion between the particle and air on heat and mass transfer is included by introducing the Nusselt number. Stripping of liquid is included at higher particle velocity. Evaporation and burning from the stripped tail are also included.

36 MATERIALS SCIENCE↗

Interaction of Burning Metal Particles

Multiple particle/droplet flames are ubiquitous in practical combustion systems, and thus the flame interaction processes are of great practical importance. This explains the strong current interest in interactive combustion phenomena. This research is aimed at the investigation of combustion parameters of microgravity model aerosols: relatively large uniform metal particles aerosolized in microgravity environment. An experiment consisting of creation and ignition of a metal multiparticle system in microgravity and high-speed video-recording of the combustion events will produce visual records of the development of individual particle flames, their interactions and the particle motion they induce simultaneously with the observation of the entire aerosol combustion process. Frame by frame analysis of the video-images taken using a high-speed movie camera will allow one to determine particle brightness temperatures and the decrease in particle diameter during combustion. Analysis of the experimental results and comparison with the results of single metal particle combustion experiments, conducted under similar microgravity conditions in the framework of a parallel program, will establish the relationship between single and multiple particle burning rates and combustion temperatures, concentrations at which the flame substructure forms rather than individual particle flames, efficiency of radiative heat transfer in metal aerosol combustion, what is the role of electrostatic forces in structuring the flame and the effect of that structure on the flame propagation rate. Although some details of fine particle aerosol clouds, such as the kinetics limited burning rate, radiative heat transfer in a system with a high specific surface, particle induced turbulence, etc., will probably not be very well simulated in the planned experiments, they are relatively well understood and can be accounted for using an adequate individual particle combustion model. On the other hand, the unknown particle interaction phenomena to be studied in this research program are generic and can be readily projected onto a cloud combustion model which would also incorporate a correction for particle size.

Dreizin, Edward L.↗

SciDAC ISEP: Integrated Simulation of Energetic Particles in Burning Plasmas

The objective of the SciDAC Center for Integrated Simulation of Energetic Particles in Burning Plasmas (ISEP) is to improve physics understanding of energetic particle (EP) confinement and EP interactions with burning thermal plasmas through large-scale simulations. The ISEP center will develop a multiscale and multiphysics ISEP framework for a predictive capability of EP physics and deliver an EP module incorporating both first-principles simulations and high fidelity reduced transport models to the fusion whole device modeling (WDM) project. The ISEP framework will enable us to perform long time, global kinetic simulations of EP physics in burning plasmas, by utilizing the full power of the next generation supercomputers. Our research and development activities will build on fruitful collaborations with computer scientists and applied mathematicians to offer enabling technologies for performance scalability, portability, solvers, coupling for integration with the fusion WDM project, and long-term preservation of data.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Interaction of Burning Metal Particles

Physical characteristics of the combustion of metal particle groups have been addressed in this research. The combustion behavior and interaction effects of multiple metal particles has been studied using a microgravity environment, which presents a unique opportunity to create an "aerosol" consisting of relatively large particles, i.e., 50-300 micrometer diameter. Combustion behavior of such an aerosol could be examined using methods adopted from well-developed single particle combustion research. The experiment included fluidizing relatively large (order of 100 micrometer diameter) uniform metal particles under microgravity and igniting such an "aerosol" using a hot wire igniter. The flame propagation and details of individual particle combustion and particle interaction have been studied using a high speed movie and video-imaging with cameras coupled with microscope lenses to resolve individual particles. Interference filters were used to separate characteristic metal and metal oxide radiation bands form the thermal black body radiation. Recorded flame images were digitized and employed to understand the processes occurring in the burning aerosol. The development of individual particle flames, merging or separation, and extinguishing as well as induced particle motion have been analyzed to identify the mechanisms governing these processes. Size distribution, morphology, and elemental compositions of combustion products were characterized and used to link the observed in this project aerosol combustion phenomena with the recently expanded mechanism of single metal particle combustion.

Dreizin, Edward L.↗

Interaction of Burning Metal Particles

Physical characteristics of the combustion of metal particle groups have been addressed in this research. The combustion behavior and interaction effects of multiple metal particles has been studied using a microgravity environment, which presents a unique opportunity to create an "aerosol" consisting of relatively large particles, i.e., 50-300 m diameter. Combustion behavior of such an aerosol could be examined using methods adopted from well-developed single particle combustion research. The experiment included fluidizing relatively large (order of 100 m diameter) uniform metal particles under microgravity and igniting such an "aerosol" using a hot wire igniter. The flame propagation and details of individual particle combustion and particle interaction have been studied using a high speed movie and video-imaging with cameras coupled with microscope lenses to resolve individual particles. Interference filters were used to separate characteristic metal and metal oxide radiation bands from the thermal black body radiation. Recorded flame images were digitized and various image processing techniques including flame position tracking, color separation, and pixel by pixel image comparison were employed to understand the processes occurring in the burning aerosol. The development of individual particle flames, merging or separation, and extinguishment as well as induced particle motion have been analyzed to identify the mechanisms governing these processes. Size distribution, morphology, and elemental compositions of combustion products were characterized and used to link the observed in this project aerosol combustion phenomena with the recently expanded mechanism of single metal particle combustion.

Dreizin, Edward L.↗

Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles: Compositions and Aging of Inorganic Particles - 2

Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

Li, Jia↗

Internal Heterogeneous Processes in Aluminum Combustion

This paper discusses the aluminum particle combustion mechanism which has been expanded by inclusion of gas dissolution processes and ensuing internal phase transformations. This mechanism is proposed based on recent normal and microgravity experiments with particles formed and ignited in a pulsed micro-arc. Recent experimental findings on the three stages observed in Al particle combustion in air and shows the burning particle radiation, trajectory (streak), smoke cloud shapes, and quenched particle interiors are summarized. During stage I, the radiation trace is smooth and the particle flame is spherically symmetric. The temperature measured using a three-color pyrometer is close to 3000 K. Because it exceeds the aluminum boiling point (2730 K), this temperature most likely characterizes the vapor phase flame zone rather than the aluminum surface. The dissolved oxygen content within particles quenched during stage I was below the detection sensitivity (about 1 atomic %) for Wavelength Dispersive Spectroscopy (WDS). After an increase in the radiation intensity (and simultaneous decrease in the measured color temperature from about 3000 to 2800 K) indicative of the transition to stage II combustion, the internal compositions of the quenched particles change. Both oxygen-rich (approx. 10 atomic %) and oxygen-lean (< 1 %) regions are identified within the particles using back-scattered electron imaging and WDS. During stage II, oscillations are observed in particle radiation and the flame and smoke cloud are distorted from their original spherically-symmetric shape. In stage III, particle radiation continues to exhibit oscillations, but its radiation intensity drops and remains at a nearly constant level. The measured temperature decreases to about 2300 K. Also, larger changes in particle velocities are observed, and oxide caps are found on quenched particle surfaces. While these results showed the correlation between the aluminum particle combustion behavior and the evolution of its internal composition, the change from the spherically symmetric to asymmetric flame shape occurring upon the transition from stage I to stage II combustion could not be understood based only on the fact that dissolved oxygen is detected in the particles. The connection between the two phenomena appeared even less significant because in earlier aluminum combustion studies carried in O2/Ar mixtures, flame asymmetry was not observed as opposed to experiments in air or O2/CO mixtures. It has been proposed that the presence of other gases, i.e., hydrogen, or nitrogen causes the change in the combustion regime.

Dreizin, E. L.↗

Internal and surface phenomena in metal combustion

Combustion of metals has been widely studied in the past, primarily because of their high oxidation enthalpies. A general understanding of metal combustion has been developed based on the recognition of the existence of both vapor-phase and surface reactions and involvement of the reaction products in the ensuing heterogeneous combustion. However, distinct features often observed in metal particle combustion, such as brightness oscillations and jumps (spearpoints), disruptive burning, and non-symmetric flames are not currently understood. Recent metal combustion experiments using uniform high-temperature metal droplets produced by a novel micro-arc technique have indicated that oxygen dissolves in the interior of burning particles of certain metals and that the subsequent transformations of the metal-oxygen solutions into stoichiometric oxides are accompanied with sufficient heat release to cause observed brightness and temperature jumps. Similar oxygen dissolution has been observed in recent experiments on bulk iron combustion but has not been associated with such dramatic effects. This research addresses heterogeneous metal droplet combustion, specifically focusing on oxygen penetration into the burning metal droplets, and its influence on the metal combustion rate, temperature history, and disruptive burning. A unique feature of the experimental approach is the combination of the microgravity environment with a novel micro-arc Generator of Monodispersed Metal Droplets (GEMMED), ensuring repeatable formation and ignition of uniform metal droplets with controllable initial temperature and velocity. The droplet initial temperatures can be adjusted within a wide range from just above the metal melting point, which provides means to ignite droplets instantly upon entering an oxygen containing environment. Initial droplet velocity will be set equal to zero allowing one to organize metal combustion microgravity experiments in a fashion similar to usual microgravity liquid fuel droplet combustion studies. In addition, the internal compositions of rapidly quenched metal particles will be analyzed using SEM technique. Such compositions are similar to those existing during the combustion and provide new insight on metal combustion processes. The results of this experimental work will be used to model the fundamental mechanisms of metal combustion. Preliminary experimental results on Al and Zr particle combustion at normal gravity are discussed here.

Dreizin, Edward L.↗

Burning rate for steel-cased, pressed binderless HMX

The burning behavior of pressed binderless HMX laterally confined in 6.4 mm i.d. steel cases was measured over the pressure range 1.45 to 338 MPa in a constant pressure strand burner. The measured regression rates are compared to those reported previously for unconfined samples. It is shown that lateral confinement results in a several-fold decrease in the regression rate for the coarse particle size HMX above the transition to super fast regression. For class E samples, confinement shifts the transition to super fast regression from low pressure to high pressure. These results are interpreted in terms of the previously proposed progressive deconsolidation mechanism. Preliminary holographic photography and closed bomb tests are also described. Theoretical one dimensional modeling calculations were carried out to predict the expected flame height (particle burn out distance) as a function of particle size and pressure for binderless HMX burning by a progressive deconsolidation mechanism.

Fifer, R. A.↗

Individual Aerosol Particles from Biomass Burning in Southern Africa: Compositions and Size Distributions of Carbonaceous Particles - 1

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

Posfai, Mihaly↗

Carbon and Hydrocarbon Particle Seeding in Air-Breathing Rotating Detonation Engine

Within the power generation community, the rotating detonation engine (RDE) is only growing in popularity with its increased performance, simple mechanism, and operation. Although significant testing is underway to characterize the RDE for integration with conventional gas turbines, this entire system is still at a relatively low technology readiness level. In the midst of RDE research, there is an initiative to understand solid particle seeding effects in the detonation performance. Under investigation at the University of Central Florida is a Department of Energy (DOE) 15.24 cm (6 in.) RDE, with a solid particle seeder in parallel with its H2 and air flow lines. Previous work on this system involved carbon particle detonation; however, the tested particles were taken one step further to include more sustainable, greener hydrocarbon particles. Testing of powdered sugar, peanut flour, and cornstarch, along with previous carbon black tests have shown not only successful detonability, but a noticeable effect on the detonation wave dynamics. Side-by-side with a particle burning model being developed, an operational map can be determined for the hydrocarbon particles particularly, which can be tuned with the local flow conditions to achieve peak operability while replacing fuels with sustainable alternatives that could even be grown.

Engineering↗

Response of convectively controlled burning to nonlinear disturbances.

A process where energy release rate is proportional to the square root of the Reynolds number of a burning particle or surface is used to demonstrate some distinctive dynamic properties of a disturbed convectively controlled burning process. The instantaneous energy release rates caused by assumed periodic flow field disturbances are numerically evaluated and examined. Correlation coefficients which express the energy released in-phase with the pressure disturbance are evaluated and analytical solutions for these coefficients are derived. The response of the process is shown to be highly sensitive to the harmonic distortion of the disturbance. For some disturbances the energy released in-phase with the pressure disturbance is an order of magnitude larger than that for linear (sinusoidal) disturbances. The results show that harmonic distortion increases the coupling between the burning process and the flow field. This amplifying effect of harmonic distortion is suppressed when a disturbance becomes steep-fronted; therefore, steepening can act to limit the equilibrium amplitudes in disturbed systems. Amplification is also suppressed when the velocity disturbance is phase shifted with respect to the pressure disturbance or when the process is exposed to a high steady velocity.

Heidmann, M. F.↗

Combustion of metal powder with dinitrogen tetroxide

In this work, we present analysis of a novel reactive material system that employs dinitrogen tetroxide (N 2 O 4 ) as a liquid oxidizer with metal powder fuels. The oxidizer was added to micron scale aluminum and zirconium powders by a remote injection system. When ignited with a high voltage spark, the mixtures were observed to possess reactivity comparable to nanocomposite reactive materials, with open-tube flame expansion velocities from 500 to 1400 m/s depending on fuel/oxidizer ratio and tube diameter. Temperatures were observed to range from 3000 to 3500 K as measured with gray body fits to 16-channel time-resolved pyrometer and time-integrated spectrometer data. These values were significantly below calculated adiabatic flame temperatures, which we attribute to local deviations from stoichiometry and kinetic/energetic limitations similar to those observed in studies of particles burning in high pressures gaseous oxidizers. Al/N 2 O 4 reactivity was found to be most likely limited by the vaporization of the metal from the particle surface and Zr/N 2 O 4 was limited by slower burning and complex interactions involving the solubility of nitrogen and oxygen in the molten Zr. We also discuss the potential for these materials to be used to create an “on/off” reactive material, since N2O4 can be added remotely and driven to evaporate via vacuum or purge of inert gases to return it to a safe condition.

36 MATERIALS SCIENCE↗