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NASA NTRS2015

Evaluation of Volatile Species in Green Monopropellant Project

NASA is interested in green monopropellants to replace hydrazine in reaction control systems (RCSs). Some current NASA programs require reduced vapor pressure and low toxicity monopropellant (green) and superior performance (specific impulse and density) formulations. Earlier vapor phase studies of a candidate green monopropellant at the NASA White Sands Test Facility (WSTF) showed the presence of a volatile species that warranted further investigation. The purpose of this study was to further characterize the volatile species and to evaluate it. The evaluation was with respect to whether the volatile species was an impurity or how it is formed, and to use that information to examine whether its presence as an impurity can be eliminated during formulation. The evaluation also considered whether formation of the volatile impurity could be prevented while not compromising the propellant. To reduce variables associated with evaluation of the propellant formulation as a whole, a precursor to one of the individual components in the propellant formulation was subjected to a NASA Standard 6001B Flammability, Off-gassing, and Compatibility Requirements and Test Procedures "Determination of Off-gassed Products (Test 7)". Testing took place in the NASA WSTF Molecular Desorption and Analysis Laboratory. One gram of the precursor was placed in a flask within a specimen container. After thermal conditioning for 72 +/- 1 h at 50 +/- 3 deg C (122 +/- 5 deg F), the atmosphere inside the specimen container was analyzed for off-gassed compounds by cryotrap gas chromatography-mass spectrometry (GC-MS) and fixed sample loop GC-flame ionization detection (GC-FID). The specimen container used was glass to minimize potential catalytic surfaces. The identification of compounds was difficult due to the complexity of the vapor phase concentrations and overlapping chromatographic peaks and mass spectra. However, eleven compounds were specifically identified and five compounds or classes of compounds were reported as unidentified. Quantitation of most of the compounds, including unidentified compounds, was as methane. Quantitating compounds or classes of compounds that were detected but for which specific calibration is not established as methane is in accordance with the Test 7 standard protocol. The thermal decomposition temperature of the precursor was significantly higher than the test temperature. Based on thermal decomposition temperature and on an examination of the structure and chemistry of the identified volatile species, the presence of the volatile species appears to be chemically reasonable with respect to the propellant formulation and is at this time attributed to impurities. Further examination of the overall propellant formulation process (including the individual components' synthesis processes) and process quality control (including purity of reagents and possible decomposition reactions) is indicated.

Greene, Benjamin↗

NASA NTRSDate not supplied

Pterodactyl: Aerodynamic and Aerothermal Modeling for a Symmetric Deployable Earth Entry Vehicle with Flaps

NASA’s Pterodactyl project has investigated a deployable atmospheric entry vehicle integrated with a flap control system that provides precision targeting during reentry. The control system consists of eight flaps mounted at the edge of a heatshield that can deflect in and out of the flow. An aerodynamic and aerothermodynamic analysis process was developed for preliminary vehicle design and aerodynamic database generation using engineering and CFD tools with varying levels of fidelity. The objective of this analysis was to: 1) understand the inherent aerodynamics, 2) provide an aerodynamics database for stability and control analysis, and 3) provide qualitative and quantitative aeroheating analysis for Thermal Protection System modeling of the flaps. A high fidelity Euler code, Cart3D, was used to resolve complex flow features such as secondary shocks and shock impingement. A wide range of supersonic (Mach 2) and hypersonic Mach numbers (up to Mach 40) were tested with an Earth atmosphere model. A process was developed to utilize the adaptive volume mesh generator utility of the perfect gas model of Cart3D to create meshes with high cell efficiency and numerical stability prior to running a 2nd order accurate solution with a real gas model. High-fidelity aerothermal CFD simulations were performed using US3D to further improve the aerothermal analysis on hypersonic flow around a complex entry vehicle shape including viscosity, chemical reactions of air species, vibrational energy, and catalytic surface reactions. In this process, it was found that the flap control system provided multi-axis control that can be utilized for entry precision targeting. Additionally, the Pterodactyl vehicle can achieve up to a trim L/D of 0.2. Finally, the increased fidelity of the aerothermal heating environments revealed that the shear stress contributes to increasing the heating on the flaps.

Deployable Entry Vehicle↗

NASA NTRSDate not supplied

Pterodactyl: Aerodynamic and Aerothermal Modeling for a Symmetric Deployable Earth Entry Vehicle with Flaps

Deployable Entry Vehicle↗

NASA NTRSDate not supplied

Thermochemical Instabilities at High Temperature Ceramic Surfaces

The surface of silicon-based high temperature ceramics exhibits thermochemical instabilities when exposed to oxygen-rich high enthalpy flows. These instabilities manifest as sudden temperature jumps of several hundred degrees and rapid material failure, when temperatures exceed 2000 K. Understanding and predicting these phenomena is critical to the design of thermal protection systems for sustained high speed flight vehicles. In this talk we review a series of test cases where surface temperature jumps were observed during plasmatron wind tunnel testing of ceramic materials, including ZrB2-SiC ultra-high temperature ceramics, C/SiC ceramic matrix composites, and silicone-based coatings for low-density carbon phenolic ablators. The underlying physical processes occurring when Si-containing ceramics are exposed to high enthalpy air flow include formation of passivating scales at low temperatures, passive to active oxidation transition, melting of oxide scales, changes in surface radiative properties, formation of porosity and changes in effective conductivity, surface catalytic recombination and transitions in catalytic properties, as well as high-temperature phase changes. The role of these processes in promoting thermochemical instabilities for the different material systems is discussed.

Ultra High Temperature Ceramics, UHTC↗

NASA NTRS1984

The role of surface generated radicals in catalytic combustion

The role of surface generated OH radicals in determining the catalytic ignition characteristics for propane oxidation on platinum were studied. The experiments were conducted in a stacked-plate, catalyst bed. Transient measurements, during catalytic ignition, of the catalyst's axial temperature profile were made and the effect of equivalence ratio, inlet temperature and inlet velocity was investigated. These measurements will provide insights which will be useful in planning and interpreting to OH measurements. Attempts to measure OH concentration in the catalyst bed using resonance absorption spectroscopy were unsuccessful, indicating that OH concentrations are below 10 to the 16th power/cc but still possibly above equilibrium values. Measurements are currently underway using forward scatter laser induced fluorescence which should extend the OH detection limits several orders of magnitude below the equilibrium concentrations.

Santavicca, D. A.↗

NASA NTRS2005

Transient Catalytic Combustor Model With Detailed Gas and Surface Chemistry

In this work, we numerically investigate the transient combustion of a premixed gas mixture in a narrow, perfectly-insulated, catalytic channel which can represent an interior channel of a catalytic monolith. The model assumes a quasi-steady gas-phase and a transient, thermally thin solid phase. The gas phase is one-dimensional, but it does account for heat and mass transfer in a direction perpendicular to the flow via appropriate heat and mass transfer coefficients. The model neglects axial conduction in both the gas and in the solid. The model includes both detailed gas-phase reactions and catalytic surface reactions. The reactants modeled so far include lean mixtures of dry CO and CO/H2 mixtures, with pure oxygen as the oxidizer. The results include transient computations of light-off and system response to inlet condition variations. In some cases, the model predicts two different steady-state solutions depending on whether the channel is initially hot or cold. Additionally, the model suggests that the catalytic ignition of CO/O2 mixtures is extremely sensitive to small variations of inlet equivalence ratios and parts per million levels of H2.

Struk, Peter M.↗

NASA NTRS1997

The Effect of Diffusional Transport and Surface Catalysis on the Aerothermodynamic Heating for Martian Atmospheric Entry

For the reentry heating of 70-degree blunt sphere-cones entering Mars at velocities in excess of 6 km/sec, a study was performed to determine the magnitude of both convective and catalytic heating on the cone forebody. Case studies of the peak heating conditions for the current NASA Mars Pathfinder entry probe, as well as the peak heating conditions of the proposed NASA Mars 2001 aerobraking orbiter mission were performed. Since the actual behavior of the chemical recombination of Mars atmosphere hypersonic shock layer species on heat shield materials is not known, and no experimental studies of any consequence have been done to determine surface reaction rates for the CO2 system, a parametric analysis of various reaction schemes and surface catalytic mechanistic models was performed. In many cases the actual Mars entry probe will have a heat shield composed of an ablative material which can either partially or completely preclude the existence of catalytic surface recombination phenomena. The extent of this blockage effect has not been examined at this time and is not considered in this effort. Instead only non-ablative computations are performed to separately evaluate the full extent of the surface catalysis and related diffusional phenomena. Parametric studies include peak heating point comparisons of non-catalytic, partially catalytic and fully catalytic total surface heat transfer for three difference surface recombination catalytic mechanisms (with and without simultaneous CO + O and O + O recombination) as well as with different species diffusion models. Diffusion model studies include constant Schmidt number (equal diffusivities) and the bifurcation, approximate multi-component diffusion model. Since the gas phase reaction kinetics for the Mars CO2 based atmosphere have also not been validated, the effect of two different (fast and slow) sets of gas kinetics on heat transfer is presented.

Henline, William D.↗

NASA NTRS1974

Interstellar molecules - Origin by catalytic reactions on grain surfaces

To determine the compound distribution formed by surface catalysis, mixtures of CO, D2, and ND2 were heated with nickel-iron or montmorillonite clay catalysts for 49-214 hours at 250 to 300 C. Compounds identified include most of the known polyatomic interstellar molecules, as well as homologous series of acetylenes, dienes, alcohols, aldehydes, ketones, ethers, esters, nitriles, amines, etc., and cyclic compounds such as furans and pyrroles. These homologous series are uniquely characteristic of surface catalysis. A search for the heavier members of these series, predicted to occur at 1/10th to 1/1,000th the abundance of the lightest members, thus comprises a crucial test of this mechanism.

Anders, E.↗

NASA NTRS1983

Orbiter catalytic/noncatalytic heat transfer as evidenced by heating to contaminated surfaces on STS-2 and STS-3

During that portion of Space Shuttle orbiter entry when significant aerodynamic heat transfer occurs, the flow over the vehicle is in chemical nonequilibrium. The parameter which most significantly influences the level of surface heat transfer in such a flow field is the catalytic efficiency of the surface with respect to the recombination of dissociated oxygen atoms. Significant, and instantaneous, changes were observed in the level of heat transfer at several lower surface centerline locations on STS-2 and STS-3. This phenomenon apparently resulted from a sudden change in the surface catalytic efficiency at these locations due to contamination of the surface by metallic oxides. As a result, data obtained from affected measurements cannot be considered as benchmark data with which to attempt to characterize nonequilibrium heat transfer to the orbiter's lower surface centerline.

Throckmorton, D. A.↗

NASA NTRS2018

Development of a Detailed Surface Chemistry Framework in DSMC

A generalized finite-rate surface chemistry framework incorporating a comprehensive list of reaction mechanisms is developed and implemented into the Direct Simulation Monte Carlo (DSMC) solver SPARTA (Stochastic PArallel Rarefied-gas Time-accurate Analyzer). The various mechanisms include adsorption, desorption, Eley-Rideal (ER), and several types of Langmuir-Hinshelwood (LH) mechanisms. The approach is to stochastically model the various competing reactions occurring on a set of active sites. Both gas-surface (e.g., adsorption, ER) and pure-surface (e.g., desorption) reaction mechanisms are incorporated, and the framework also includes catalytic or surface altering mechanisms involving the participation of the bulk-phase species (e.g., bulk carbon atoms). Marschall and MacLean developed a general formulation in which multiple phases and surface sites are used and a similar convention is adopted in the current work. Expressions for the microscopic parameters of reaction probabilities (for gas-surface reactions) and frequencies (for pure-surface reactions) that are required for DSMC are derived from the surface properties and macroscopic parameters such as rate constants, sticking coefficients, etc. The energy and angular distributions of the products are specified according to the reaction type and input parameters. This framework also presents physically consistent procedures to accurately compute the reaction probabilities and frequencies in the case of multiple reactions. The result is a modeling tool with a wide variety of surface reactions characterized via user-specified reaction rate constants, surface properties and parameters.

Surface Chemistry↗

NASA NTRS2017

Development of a Detailed Surface Chemistry Framework in DSMC

Many of the current direct simulation Monte Carlo (DSMC) codes still employ only simple surface catalysis models. These include only basic mechanisms such as dissociation, recombination, and exchange reactions, without any provision for adsorption and finite rate kinetics. Incorporating finite rate chemistry at the surface is increasingly becoming a necessity for various applications such as high speed re-entry flows over thermal protection systems (TPS), micro-electro-mechanical systems (MEMS), surface catalysis, etc. In the recent years, relatively few works have examined finite-rate surface reaction modeling using the DSMC method.In this work, a generalized finite-rate surface chemistry framework incorporating a comprehensive list of reaction mechanisms is developed and implemented into the DSMC solver SPARTA. The various mechanisms include adsorption, desorption, Langmuir-Hinshelwood (LH), Eley-Rideal (ER), Collision Induced (CI), condensation, sublimation, etc. The approach is to stochastically model the various competing reactions occurring on a set of active sites. Both gas-surface (e.g., ER, CI) and pure-surface (e.g., LH, desorption) reaction mechanisms are incorporated. The reaction mechanisms could also be catalytic or surface altering based on the participation of the bulk-phase species (e.g., bulk carbon atoms). Marschall and MacLean developed a general formulation in which multiple phases and surface sites are used and we adopt a similar convention in the current work. Microscopic parameters of reaction probabilities (for gas-surface reactions) and frequencies (for pure-surface reactions) that are require for DSMC are computed from the surface properties and macroscopic parameters such as rate constants, sticking coefficients, etc. The energy and angular distributions of the products are decided based on the reaction type and input parameters. Thus, the user has the capability to model various surface reactions via user-specified reaction rate constants, surface properties and parameters.

Gas↗

NASA NTRS2009

Boundary Layer Protuberance Simulations in Channel Nozzle Arc Jet

Various protuberance heights and shapes were modeled in the channel nozzle of the NASA Johnson Space Center Atmospheric Reentry Materials and Strictures Facility with the Data- Parallel Line Relaxation computational fluid dynamics code. The heating on the protuberance was compared to baseline (no protuberance) heating at a single fixed arc jet condition in order to obtain heating augmentation factors that will be used for flight traceability in the Boundary Layer Transition Flight Experiment on Space Shuttle Orbiter flights STS-119 (completed) and STS-128 (future flight). The arc jet simulations were performed in conjunction with the actual ground tests performed on the flight version (selected height and shape) of the protuberance. Thearc jet simulations for the final (flight version) protuberance included non-uniform inflow conditions beginning at the channel nozzle throat. The 2D inflow condition was modeled based on the current best practices methodology and used variable enthalpy and mass flow rate across the throat. Channel walls were modeled as fully catalytic isothermal surfaces, while the test section (consisting of Reaction Cured Glass tiles) was modeled as a partially catalytic radiative equilibrium wall. The results of the protuberance and baseline simulations were compared to the applicable ground test results. In addition, the obtained heating augmentation factors were compared to the factors derived from the STS-119 flight data. The effects of the protuberance shock on the opposite channel wall were also investigated.

Larin, M. E.↗

NASA NTRS2010

Boundary Layer Protuberance Simulations in Channel Nozzle Arc-Jet

Two protuberance designs were modeled in the channel nozzle of the NASA Johnson Space Center Atmospheric Reentry Materials and Structures Facility with the Data-Parallel Line Relaxation computational fluid dynamics code. The heating on the protuberance was compared to nominal baseline heating at a single fixed arc-jet condition in order to obtain heating augmentation factors for flight traceability in the Boundary Layer Transition Flight Experiment on Space Shuttle Orbiter flights STS-119 and STS-128. The arc-jet simulations were performed in conjunction with the actual ground tests performed on the protuberances. The arc-jet simulations included non-uniform inflow conditions based on the current best practices methodology and used variable enthalpy and constant mass flow rate across the throat. Channel walls were modeled as fully catalytic isothermal surfaces, while the test section (consisting of Reaction Cured Glass tiles) was modeled as a partially catalytic radiative equilibrium wall. The results of the protuberance and baseline simulations were compared to the applicable ground test results, and the effects of the protuberance shock on the opposite channel wall were investigated.

Marichalar, J. J.↗

NASA NTRS1980

Catalytic recombination of nitrogen and oxygen on high-temperature reusable surface insulation

The energy transfer catalytic recombination coefficient for nitrogen and oxygen recombination on the surface coating of high-temperature reusable surface insulation (HRSI) is inferred from stagnation point heat flux measurements in a high-temperature dissociated arc jet flow. The resulting catalytic recombination coefficients are correlated with an Arrhenius model for convenience, and these expressions may be used to account for catalytic recombination effects in predictions of the heat flux on the HRSI thermal protection system of the Space Shuttle Orbiter during reentry flight. Analysis of stagnation point pressure and total heat balance enthalpy measurements indicates that the arc heater reservoir conditions are not in chemical equilibrium. This is contrary to what is usually assumed for arc jet analysis and indicates the need for suitable diagnostics and analyses, especially when dealing with chemical reaction phenomena such as catalytic recombination heat transfer effects.

Scott, C. D.↗

NASA NTRS1973

Arc jet tests of RSI materials: Screening and comparative evaluation

Cyclic convective heating test results show that all surface insulation materials tested exhibit a wide range of surface emittance and catalytic activity depending on their surface coatings. Coatings have a significant effect on the overall material response depending on boundary layer characteristics.

Schaefer, J. W.↗

NASA NTRS1995

Dual-Code Solution Strategy for Chemically-Reacting Hypersonic Flows

A new procedure seeks to combine the thin-layer Navier-Stokes solver LAURA with the parabolized Navier-Stokes solver UPS for the aerothermodynamic solution of chemically-reacting air flow fields. The interface protocol is presented and the method is applied to two slender, blunted shapes. Both axisymmetric and three-dimensional solutions are included with surface pressure and heat transfer comparisons between the present method and previously published results. The case of Mach 25 flow over an axisymmetric six degree sphere-cone with a non-catalytic wall is considered to 100 nose radii. A stability bound on the marching step size was observed with this case and is attributed to chemistry effects resulting from the non-catalytic wall boundary condition. A second case with Mach 28 flow over a sphere-cone-cylinder-flare configuration is computed at both two and five degree angles of attack with a fully-catalytic wall. Surface pressures are seen to be within five percent with the present method compared to the baseline LAURA solution and heat transfers are within 10 percent. The effect of grid resolution is investigated in both the radial and streamwise directions. The procedure demonstrates significant, order of magnitude reductions in solution time and required memory for the three-dimensional case in comparison to an all thin-layer Navier-Stokes solution.

Wood, William A.↗

NASA NTRS1995

Formation of Hydrocarbons in the Outflows from Red Giants

The formation of hydrocarbons in the oxygen-rich outflows from red giants was studied. The existence of organic molecules in such outflows has been known for several years; however, their surprisingly high abundances has been a mystery since all of the carbon had been thought to be irretrievably locked up in CO, the most strongly bound molecule. CO is the first molecule to form from the atoms present in the star's extended atmosphere, and as strong stellar winds drive a cooling outflow, dust grains condense out. In oxygen-rich outflows, the dust is thought to be composed mainly of silicates and other metal oxides. Perhaps the noble metals can condense out in metallic form, in particular the relatively abundant transition metals iron and nickel. We proposed that perhaps the carbon reservoir held as CO can be accessed through a catalytic process involving the chemisorption of CO and H2 onto grains rich in metallic iron. CO and H2 are the two most abundant molecules in circumstellar outflows, and they both are known to dissociate on transition metal surfaces at elevated temperatures, freeing carbon to form organic molecules such as methane. We believe methane is a precursor molecule to the organics observed in oxygen-rich red giants. We have developed a nonequilibrium numerical model of a surface chemical (catalytic) process. Based on this model, we believe that methane can be formed under the conditions present in circumstellar outflows. Although the methane formation rates are exceptionally low under these conditions, over dynamical timescales, a significant amount of CO can be converted to methane and driven further out in the envelope, explaining the presence of organics there.

Roberge, Wayne↗

NASA NTRS2010

High efficiency tantalum-based ceramic composite structures

Tantalum-based ceramics are suitable for use in thermal protection systems. These composite structures have high efficiency surfaces (low catalytic efficiency and high emittance), thereby reducing heat flux to a spacecraft during planetary re-entry. These ceramics contain tantalum disilicide, molybdenum disilicide and borosilicate glass. The components are milled, along with a processing aid, then applied to a surface of a porous substrate, such as a fibrous silica or carbon substrate. Following application, the coating is then sintered on the substrate. The composite structure is substantially impervious to hot gas penetration and capable of surviving high heat fluxes at temperatures approaching 3000.degree. F. and above.

Stewart, David A.↗