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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
NASA NTRS2009

Life on Mars: Evidence from Martian Meteorites

New data on martian meteorite 84001 as well as new experimental studies show that thermal or shock decomposition of carbonate, the leading alternative non-biologic explanation for the unusual nanophase magnetite found in this meteorite, cannot explain the chemistry of the actual martian magnetites. This leaves the biogenic explanation as the only remaining viable hypothesis for the origin of these unique magnetites. Additional data from two other martian meteorites show a suite of biomorphs which are nearly identical between meteorites recovered from two widely different terrestrial environments (Egyptian Nile bottomlands and Antarctic ice sheets). This similarity argues against terrestrial processes as the cause of these biomorphs and supports an origin on Mars for these features.

McKay, David S.↗
DOE OSTI2021

Shock tube investigation of high-temperature, extremely-rich oxidation of several co-optima biofuels for spark-ignition engines

To reduce the reliance on fossil fuels in the transportation sector and increase combustion efficiency, the Co-Optima initiative from US Department of Energy identified the top 10 biofuels for downsized, boosted, spark-ignition engines. Most of these biofuels have detailed reaction mechanisms available in literature developed based on studies at temperatures lower than 1700 K and an equivalence ratio of less than five. As such, the performance of these detailed mechanisms at high temperature and extremely rich conditions are unknown. It is important to validate kinetic mechanisms at these conditions because they are conducive to soot formation. Prediction of soot by chemical kinetic models relies on the prediction of underlying benchmark species like carbon monoxide and ethylene. In this work, we conduct high temperature (1700–2050 K) and high equivalence ratio(Φ=8.6) oxidation of these biofuels, namely 2,4,4-trimethyl-1-pentene (α-diisobutylene), ethanol, cyclopentanone, methyl acetate, and 2-methylfuran, blended in ethylene behind reflected shock waves at 4–4.7 atm pressure. Carbon monoxide and ethylene time histories are measured simultaneously using a continuous feedback quantum cascade laser near 4.9 µm and a tunable CO 2 gas laser at 10.532 nm, respectively. Results show that ethanol blend forms more carbon monoxide than other biofuels and consumes ethylene faster than the biofuel blends in the temperature range considered. Overall, the performance of different mechanisms in literature are evaluated against the experimental results. The novel reaction mechanism ‘the Co-Optima model’, which includes the sub mechanisms for all the biofuels in this study, was found to be the best mechanism for the experimental conditions studied.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

An experimental and kinetic modeling study of the pyrolysis of isoprene, a significant biogenic hydrocarbon in naturally occurring vegetation fires

Isoprene dominates the carbon flux emitted by vegetation and constitutes 40% of non-methane biogenic emissions worldwide. Despite pyrolysis experiments at temperatures above 1000 K showing a link between isoprene combustion and aromatic species formation, comprehensive mechanistic research on isoprene is scarce in the literature. Here, in this work, we carry out an experimental and theoretical study to build, for the first time, a chemical kinetic model describing isoprene pyrolysis. The formation of polycyclic aromatic hydrocarbon (PAH) precursor species, often observed in vegetation fire plumes, is partially explained by isoprene pyrolysis experiments and theoretical modeling. Molecular dynamics (MD) simulations unveil reaction pathways from allylic isoprenyl radicals to allene and cyclopentadiene (CPD) intermediates, two relevant species detected in the experiments. Rate constants for these identified pathways are calculated using variational transition state theory to update the kinetic model, which is validated against single-pulse shock tube (SPST), and jet-stirred reactor (JSR) experimental data in the temperature range of 850–1690 K. The kinetic model presents satisfactory agreement with the SPST experimental data, and a reaction pathway analysis shows that association of propargyl radicals results in benzene formation. The JSR pathway analysis also identifies the prominent reactions for CPD, benzene, styrene, and toluene formation. Our model does not reproduce the CPD experimental profiles, indicating that additional studies are necessary. Overall, our findings advance the understanding of isoprene pyrolysis and its related atmospheric pollutants in naturally occurring vegetation fires where smoldering and oxygen-deficient combustion processes are present.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Synthesizing Carbon‐Supported, High‐Loading, Ultra‐Small Pt 3 Ni Nanoparticles via Tuning the Surface Electrostatic Effect

Carbon‐supported nanoparticles (NPs) are widely used as catalysts in fuel cells and electrolyzers. While it is well known that NPs with smaller size and higher loading often lead to better catalytic activity, they remain challenging to synthesize due to the weak control over the surface properties of the support. Herein, a facile approach to synthesize carbon‐supported, high‐loading, and ultra‐small Pt 3 Ni NPs via applying thermal shock on strongly interacted carbon support with metal salt is reported. Specifically, sodium citrate is introduced into the precursor solution and substrate mixture, which induces strong electrostatic effect between metal salts and carbon particles that markedly improves precursor anchoring and dispersion, thereby achieving high particle loading as well as small size and distribution. As a proof‐of‐concept, the synthesis of Pt 3 Ni NPs supported on carbon black with particle size of 1.56 ± 0.36 nm at 30 wt% loading and 1.66 ± 0.56 nm at 40 wt% loading is reported, where the sizes are among the smallest while the loadings are among the highest in the literature. This approach can be readily extended to many compositions and substrates, with tunable particle size and loading, thereby substantially expanding the synthesis space for NP catalysts in various electrochemical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Fact Sheet: Range Complex

NASA Ames has a long tradition in leadership with the use of ballistic ranges and shock tubes for the purpose of studying the physics and phenomena associated with hypervelocity flight. Cutting-edge areas of research run the gamut from aerodynamics, to impact physics, to flow-field structure and chemistry. This legacy of testing began in the NACA era of the 1940's with the Supersonic Free Flight Tunnel, and evolved dramatically up through the late 1950s with the pioneering work in the Ames Hypersonic Ballistic Range. The tradition continued in the mid-60s with the commissioning of the three newest facilities: the Ames Vertical Gun Range (AVGR) in 1964, the Hypervelocity Free Flight Facility (HFFF) in 1965 and the Electric Arc Shock Tube (EAST) in 1966. Today the Range Complex continues to provide unique and critical testing in support of the Nation's programs for planetary geology and geophysics; exobiology; solar system origins; earth atmospheric entry, planetary entry, and aerobraking vehicles; and various configurations for supersonic and hypersonic aircraft.

Cornelson, C.↗
DOE OSTI2020

Shock Hugoniot measurements of single-crystal 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) compressed to 83 GPa

We present laser-driven shock Hugoniot measurements of single-crystal (SC) 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) between 15 and 83 GPa, spanning pressures below and well above the Chapman–Jouguet pressure of ~28 GPa for TATB formulations (TATB grains mixed with plastic binders at 5–10 wt. %). The new SC data are generally ~3% more compressible than previously published data on neat and formulated TATB measured in gas-gun and explosive-driven experiments. An exception is at compressions in the density of ~1.5 (~30–40 GPa), where our new SC data exhibit significantly lower pressures than previous results on overdriven TATB formulations, suggesting that our SC samples remain largely unreacted below 35 GPa over the short nanosecond-time scales inherent to our laser-driven experiments. We report these novel equation-of-state measurements are a critical step toward understanding TATB in its most fundamental form and improving predictive modeling of TATB-based explosives.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Highly ordered graphite (HOPG) to hexagonal diamond (lonsdaleite) phase transition observed on picosecond time scales using ultrafast x-ray diffraction

Here, the response of rapidly compressed highly oriented pyrolytic graphite (HOPG) normal to its basal plane was investigated at a pressure of ~80 GPa. Ultrafast x-ray diffraction using ~100 fs pulses at the Materials Under Extreme Conditions sector of the Linac Coherent Light Source was used to probe the changes in crystal structure resulting from picosecond timescale compression at laser drive energies ranging from 2.5 to 250 mJ. A phase transformation from HOPG to a highly textured hexagonal diamond structure is observed at the highest energy, followed by relaxation to a still highly oriented, but distorted graphite structure following release. We observe the formation of a highly oriented lonsdaleite within 20 ps, subsequent to compression. This suggests that a diffusionless martensitic mechanism may play a fundamental role in phase transition, as speculated in an early work on this system, and more recent static studies of diamonds formed in impact events.

58 GEOSCIENCES↗
NASA NTRS1977

Computational models for the analysis of three-dimensional internal and exhaust plume flowfields

This paper describes computational procedures developed for the analysis of three-dimensional supersonic ducted flows and multinozzle exhaust plume flowfields. The models/codes embodying these procedures cater to a broad spectrum of geometric situations via the use of multiple reference plane grid networks in several coordinate systems. Shock capturing techniques are employed to trace the propagation and interaction of multiple shock surfaces while the plume interface, separating the exhaust and external flows, and the plume external shock are discretely analyzed. The computational grid within the reference planes follows the trace of streamlines to facilitate the incorporation of finite-rate chemistry and viscous computational capabilities. Exhaust gas properties consist of combustion products in chemical equilibrium. The computational accuracy of the models/codes is assessed via comparisons with exact solutions, results of other codes and experimental data. Results are presented for the flows in two-dimensional convergent and divergent ducts, expansive and compressive corner flows, flow in a rectangular nozzle and the plume flowfields for exhausts issuing out of single and multiple rectangular nozzles.

Dash, S. M.↗
NASA NTRS1971

Ablation and radiation coupled viscous hypersonic shock layers, volume 1

The results for a stagnation-line analysis of the radiative heating of a phenolic-nylon ablator are presented. The analysis includes flow field coupling with the ablator surface, equilibrium chemistry, a step-function diffusion model and a coupled line and continuum radiation calculation. This report serves as the documentation, i e. users manual and operating instructions for the computer programs listed in the report.

Engel, C. D.↗
DOE OSTI2021

Tailoring the Local Environment of Platinum in Single-Atom Pt 1 /CeO 2 Catalysts for Robust Low-Temperature CO Oxidation

A single-atom Pt 1 /CeO 2 catalyst formed by atom trapping (AT, 800 degrees C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over-stabilization of Pt 2+ in a highly symmetric square-planar Pt 1 O 4 coordination environment. Reductive activation to form Pt nanoparticles (NPs) results in enhanced activity; however, the NPs are easily oxidized, leading to drastic activity loss. In this work, we show that tailoring the local environment of isolated Pt 2+ by thermal-shock (TS) synthesis leads to a highly active and thermally stable Pt 1 /CeO 2 catalyst. Ultrafast shockwaves (>1200 degrees C) in an inert atmosphere induced surface reconstruction of CeO 2 to generate Pt single atoms in an asymmetric Pt 1 O 4 configuration. Owing to this unique coordination, Pt 1 δ+ in a partially reduced state dynamically evolves during CO oxidation, resulting in exceptional low-temperature performance. CO oxidation reactivity on the Pt 1 /CeO 2 _TS catalyst was retained under oxidizing conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Many-body reactive force field development for carbon condensation in C/O systems under extreme conditions

In this paper, we describe the development of a reactive force field for C/O systems under extreme temperatures and pressures, based on the many-body Chebyshev Interaction Model for Efficient Simulation (ChIMES). The resulting model, which targets carbon condensation under thermodynamic conditions of 6500 K and 2.5 g cm –3 , affords a balance between model accuracy, complexity, and training set generation expense. We show that the model recovers much of the accuracy of density functional theory for the prediction of structure, dynamics, and chemistry when applied to dissociative condensed phase systems at 1:1 and 1:2 C:O ratios, as well as molten carbon. Our C/O modeling approach exhibits a 104 increase in efficiency for the same system size (i.e., 128 atoms) and a linear system size scalability over standard quantum molecular dynamics methods, allowing the simulation of significantly larger systems than previously possible. We find that the model captures the condensed-phase reaction-coupled formation of carbon clusters implied by recent experiments, and that this process is susceptible to strong finite size effects. Overall, we find the present ChIMES model to be well suited for studying chemical processes and cluster formation at pressures and temperatures typical of shock waves. We expect that the present C/O modeling paradigm can serve as a template for the development of a broader high pressure–high temperature force-field for condensed phase chemistry in organic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Synthesis and investigation into explosive sensitivity for a series of new picramide explosives

Tailoring the molecular properties that govern energetic material sensitivity is essential to improve safety and help develop new energetic materials. Despite this need, understanding the complex chemistry and physics of explosive initiation and propagation is still a challenge. Recent work by our group has reinforced the view that explosive sensitivity under sub-shock conditions is connected to the strength of the weakest covalent bond in the molecule, that is, its “trigger linkage.” These correlations have been observed with different classes of energetic molecules and indicate that “trigger linkage” bond breaking, and heat of explosion are good indicators for the sensitivity trends. Herein we report the synthesis of aliphatic energetic materials with ethane, propane and neopentane backbones. Experimental and computational studies show that the trigger linkage model, based on results from quantum molecular dynamics simulations, correctly predicts trends observed in the impact sensitivity of the molecules. However, while the model predicts the impact sensitivities of the ethane series, the neopentane series has higher impact sensitivities than predicted, which is presumably influenced by crystal packing effects.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Anisotropic Hot Spot Formation at a Grain Boundary in Shock-Compressed TATB High Explosive Crystal

Secondary high explosives (HEs) exhibit rich microstructure that promotes the formation of hot spots responsible for detonation initiation, but the role of microstructural interfaces remains poorly quantified. To this end, we develop extensions for the generalized crystal-cutting method (GCCM) to prepare molecular dynamics (MD) simulation cells containing grain boundaries (GBs) and other crystal–crystal interfaces with prescribed tilt and twist orientations. Using the GCCM, we perform MD simulations of shock interactions with a GB between the (001) and (100) crystal facets in the secondary HE TATB (1,3,5-triamino-2,4,6-trinitrobenzene). Our MD simulations reveal a strong directional dependence to the formation of a hot spot at the GB interface. In particular, transmission of the shock from the (001) grain to the (100) grain yields a hot spot in the (100) grain at the GB interface, whereas no hot spot is produced when an equivalent shock transits the GB in the opposite direction. We trace the origin of this GB anisotropy to three dominant factors: (1) the intrinsic differences in shock-deformation mechanisms and wave structures for the bulk (100) and (001) grains, which leads to distinct geometries and mechanical impedances upon shock arrival to the GB depending on which grains are donor or acceptor for the transmitted shock; (2) the different time intervals separating the initial shock rise and the formation of steady wave structures in the respective donor–acceptor configurations; and (3) the differences in time scales required to re-establish local thermal equilibrium. Interfacial hot spots form when these factors combine to impede development of a steady two-wave structure and instead induce a localized, pseudosingly shocked region that undergoes a higher rate of work production (resulting in a higher temperature) compared to when the steady two-wave structure develops further from the interface. The extensions to the GCCM approach presented here are anticipated to facilitate a wide range of MD studies that focus on understanding the role of crystal–crystal interfaces in molecular materials.

organic↗
NASA NTRS1989

Experimental and computational results for 5 degree blunt cones with shock generators at high velocity

Experiments and computations have been performed under laminar conditions in air on 5-deg blunt cones at velocities of 5 km/s and 6 km/s and at Reynolds numbers of 100,000 and 1 million. The computations were performed using ideal-, equilibrium- and nonequilibrium-chemistry models for air. At the conditions of the tests, the aerodynamic coefficients are sensitive to the real-gas effects present, and both experimental and computational aerodynamic coefficients show real-gas and nonlinear effects. The nonequilibrium computations show that a large amount of oxygen is dissociated in the blunt nose region of the flow and much of the oxygen remains dissociated over the entire length of the body, providing an insight into the source of the observed effects in the aerodynamic coefficients. The experimental and computational shock-shapes are in good agreement.

Strawa, A. W.↗
DOE OSTI2023

Multiscale Reactive Model for 1,3,5-Triamino-2,4,6-trinitrobenzene Inferred by Reactive MD Simulations and Unsupervised Learning

When high-energy-density materials are subjected to thermal or mechanical insults at extreme conditions (shock loading), a coupled response between the thermo-mechanical and chemical behaviors is systematically induced. Herein we develop a reaction model for the fast chemistry of 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) at the mesoscopic scale, where the chemical behavior is determined by underlying microscopic reactive simulations. The slow carbon cluster formation is not discussed in the present work. All-atom reactive molecular dynamics (MD) simulations are performed with the ReaxFF potential, and a reduced-order chemical kinetics model for TATB is fitted to isothermal and adiabatic simulations of single crystal chemical decomposition. Unsupervised machine learning techniques based on non-negative matrix factorization are applied to MD trajectories to model the decomposition kinetics of TATB in terms of a four-component model. The associated heats of reaction are fit to the temperature evolution from adiabatic decomposition trajectories. Using a chemical species analysis, we show that non-negative matrix factorization captures the main chemical decomposition steps of TATB and provides an accurate estimation of their evolution with temperature. The final analytical formulation, coupled to a diffusion term, is incorporated into a continuum formalism, and simulation results are compared one-to-one against MD simulations of 1D reaction propagation along different crystallographic directions and with different initial temperatures. A good agreement is found for both the temporal and spatial evolution of the temperature field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1988

An analytical study of the hydrogen-air reaction mechanism with application to scramjet combustion

A chemical kinetic mechanism for the combustion of hydrogen has been assembled and optimized by comparing the observed behavior as determined in shock tube and flame studies with that predicted by the mechanism. The reactions contained in the mechanism reflect the current state of knowledge of the chemistry of the hydrogen/air system, and the assigned rate coefficients are consistent with accepted values. It was determined that the mechanism is capable of satisfactorily reproducing the experimental results for a range of conditions relevant to scramjet combustion. Calculations made with the reaction mechanism for representative scramjet combustor conditions at Mach 8, 16, and 25 showed that chemical kinetic effects can be important and that combustor models which use nonequilibrium chemistry should be used in preference to models that assume equilibrium chemistry. For the conditions examined the results also showed the importance of including the HO2 chemistry in the mechanism. For Mach numbers less than 16, the studies suggest that an ignition source will most likely be required to overcome slow ignition chemistry. At Mach 25, the initial temperature and pressure was high enough that ignition was rapid and the presence of an ignition source did not significantly affect reaction rates.

Jachimowski, Casimir J.↗
NASA NTRS1978

West Clearwater, Quebec impact structure. I - Field geology, structure and bulk chemistry. II - Petrology

A field study at the 30-km-diameter West Clearwater impact crater was carried out during the summer of 1977 to identify the nature of the flow of impact melt and less shocked debris during the excavation stage of the cratering process. The present paper investigates: (1) comparisons with other impact craters and lunar samples; (2) generation and emplacement mechanisms of impact melts and associated clastic debris; and (3) the geometry of the transient cavity and the pristine morphology of the crater.

Simonds, C. H.↗