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DOE OSTI2021

Rock Fracturing Using High-Pressure Ethylene/Nitrous Oxide Detonations

The present work investigates high initial pressure detonations of a stoichiometric mixture of ethylene and nitrous oxide (C2H4 + 6N2O) as a method of fracturing rock beneath the ground surface. These tests were conducted at a test site operated by the Energetic Materials Research and Testing Center (EMRTC), Socorro, New Mexico. The volume under the surface used for testing (called the Down Hole Assembly) consists of a 0.438 in. ID x 50 ft. long stainless-steel tube running down from the test site to a well bore which is 3 in. ID x 10 ft. long and the rock in the well bore is exposed to the propagating combustion wave. The testing carried out at Zucrow Laboratories in the smaller, alloy steel combustion vessel provided a scaling of pressures expected in the well bore. The combustion is initiated by energizing an EBW (Exploding Bridge Wire) above the ground surface. The experimental setup accommodates one high pressure (100,000 psia) transducer to measure the pressure peak and is placed approximately 5 ft. above the ground surface and 5 ft. downstream of the EBW. The focus of this series of experiments is to investigate the dependence of fracture to the rock beneath the surface on initial pressures of the mixture of ethylene and nitrous oxide. Experiments were carried out at initial pressures varying between 125 psia and 300 psi. The transducer recorded elevated pressures, which were 2.3 to 2.6 times in excess of the CJ values. The experimental results are discussed and explained in this report.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Experimental Measurements of Soot and Soot Precursors of Sustainable Aviation Fuels

Sustainable Aviation Fuels (SAFs) are promising for decarbonizing the challenging-to-electrify aerospace sector and reducing yearly greenhouse gas emissions by thousands of tons. Developing predictive detailed chemical kinetic models for SAF (and traditional) fuel mixtures necessitates a robust experimental database to elucidate the intricate pyrolysis and oxidation chemistry of SAF fuel blend components. Two critical components of SAF surrogate mixtures are iso-dodecane isomers and trans-decalin. This report characterizes the structure of three slightly sooting, laminar, non-premixed, nitrogen-diluted Planar Mixing Layer Flames (PMLFs) fueled by either pure ethylene, ethylene doped with 1500ppm of either 2,2,4,6,6-pentamethyl-heptane or trans-decalin. The flames have the same stoichiometric mixture fraction and total mole fraction of fuels in the fuel stream (X F,F = X C2H4,F + X Dopant,F = 0.26), resulting in approximately the same maximum temperature (T max ≈ 1800 K) to highlight the effect of doping on soot and its gaseous precursors. The PMLF is unconfined and established between adjacent planar jets of the fuel and oxidizer streams surrounded by annular shielding nitrogen. The flow is stabilized by exhausting the hot buoyant flame products through a slot in a downstream plate onto which the cold flow impinges. Importantly, any horizontal cross-section of the PMLF has a self-similar thermochemical structure of a reactive boundary layer that grows at increasing Height Above the Burner (HAB). Therefore, the horizontal cross-sections of a PMLF can be modeled as a One-Dimensional Counterflow Flame (1D-CF) with very low strain rates which are unachievable in traditional CFs and yield a structure that is several millimeters thick. In brief, the PMLF is ideal for performing spatially resolved measurements with minimal effects of the sampling-induced perturbations, to develop and validate detailed chemical kinetic models on time scales of a few tens of milliseconds that are relevant in aviation applications. The horizontal profiles of C0-C18 gaseous species at HAB = 50 mm and soot volume fraction at 25 and 50 mm are measured using capillary sampling followed by GC-MS analyses and Laser Induced Emission Spectroscopy (LIES), respectively. Additionally, the Elastic Laser Light Scattering (E-LLS) coefficient is measured at HAB = 50 mm and 25 mm to determine the strain rates of the 1D-CFs equivalent to the characterized PMLF horizontal cross sections and the profile of the E-LLS equivalent diameter of soot. The comparison of the results in the base PMLF fueled only by ethylene with those in either doped PMLF in which 1500 ppm of ethylene are replaced with 2,2,4,6,6-pentamethyl-heptane or trans-decalin, reveals that the doping increases the mole fraction of several Polycyclic Aromatic Hydrocarbons (PAHs) at both HABs by a factor of approximately 2.5, and the soot volume fraction at both HABs by factors of ~1.5 for 2,2,4,6,6-pentamethyl-heptane and ~1.25 for trans-decalin doping, respectively. Conversely, doping causes a near doubling of the soot equivalent diameter only at HAB = 50 mm, without significant effects at 25 mm. The experimental results partially validate the tested state-of-the-art detailed chemical kinetic model and also point toward the further improvement of its predictive capabilities.

10 SYNTHETIC FUELS↗

DOE OSTI2025

High Pressure Measurement of Soot Formation Applicable to Energetic Materials Fireballs

The addition of hydrogen and oxygen to a hydrocarbon fuel mixture has a significant effect on its sooting tendencies at high pressures. Understanding the mechanism behind the formation of soot is key to proper chemical modeling of fireballs. The objective of this research is to investigate formation rates and soot induction times of intermediary chemicals resulting from energetic material combustion. Three intermediaries, acetylene (C2H2), ethylene (C2H4), and propyne (C3H4-P) are studied. Here, a laser spectroscopy system was utilized to measure soot formation, induction time, and detail the time histories of soot experiments performed using the University of Central Florida high pressure shock tube facility.

Loye, Timothy [University of Central Florida, Orla↗

NASA NTRS1972

Evaluation of advanced bladder technology

Research conducted during this period is reported. Studies presented include: (1) diffusion and permeation of CO2, O2, N2, and NO2 through polytetra fluoroethylene; (2) diffusion, permeation and solubility of simple gases (CO2, O2, N2, CH4, C2H6, C3H8, and C2H4) through a copolymer of hexafluoro propylene and tetrafluoro ethylene (FEP); (3) viscous flow and diffusion of gases throug small apertures; (4) diffusion and permeation of O2, N2, CO2, CH4, C2H6, and C3H8 through nitroso rubber; and (5) results of gas transport studies with carborane siloxane, nitroso rubber, silicone membrane, krytox coating on teflon, and FEP coated glass cloth. Publications generated under this program are listed.

Christensen, M. V.↗

NASA NTRS1972

Simple technique for sequential Q-switching of molecular lasers.

A simple technique for sequentially Q-switching molecular lasers is discussed in which an optical scanner is used as an optical folding element in a laser cavity consisting of a stationary diffraction grating and partially reflecting mirror. Sequential Q-switching of a conventional CO2 laser is demonstrated in which over sixty-two transitions between 9.2 and 10.8 microns are observed. Rapid repetition rates (200 Hz) and narrow laser pulses (less than 5 microsec) allow conventional signal processing techniques to be used with this multiwavelength laser source which is a versatile tool for laser propagation studies, absorption spectroscopy, and gain measurements. Results of a preliminary experiment demonstrating the utility of measuring selective absorption of CO2 laser wavelengths by C2H4 are shown.

Lucht, R. A.↗

NASA NTRS1973

Carbon chemistry of Luna 16 and Luna 20 samples.

Luna 16 and Luna 20 samples were analyzed for volatilizable species using vacuum pyrolysis to 1400 C. The major gaseous products evolved (ranging from 10-650 micrograms/g) were H2O, CO, CO2, N2 and CH4. Minor components (all less than 10 micrograms/g) included NH3, HCN, NO, SO2, H2S, C2H2, C2H4, C2H6, C3H6 and higher hydrocarbons, benzene, toluene, and the polymeric contaminants Teflon and silicone oil. The total carbon and nitrogen contents (micrograms/g) for these sieved samples were: Luna 16 - C 418, N 134 and Luna 20 - C 380, N 80.

Simoneit, B. R.↗

NASA NTRS1976

Shear strength of metal-sapphire contacts

The shear strength of polycrystalline Ag, Cu, Ni, and Fe contacts on clean (0001) sapphire has been studied in ultrahigh vacuum. Both clean metal surfaces and surfaces exposed to O2, Cl2, and C2H4 were used. The results indicate that there are two sources of strength of Al2O3-metal contacts: an intrinsic one that depends on the particular clean metal in contact with Al2O3 and an additional one due to intermediate films. The shear strength of the clean metal contacts correlated directly with the free energy of oxide formation for the lowest metal oxide, in accord with the hypothesis that a chemical bond is formed between metal cations and oxygen anions in the sapphire surface. Contacts formed by metals exposed to chlorine exhibited uniformly low shear strength indicative of van der Waals bonding between chlorinated metal surfaces and sapphire. Contacts formed by metals exposed to oxygen exhibited enhanced shear strength, in accord with the hypothesis that an intermediate oxide layer increases interfacial strength.

Pepper, S. V.↗

NASA NTRS1977

Reforming of glucose and wood at the critical conditions of water

Reforming of organics in aqueous solutions is being investigated as a potential waste treatment process. Earlier studies showed that glucose in water reacts to form a gaseous mixture of CO, H2, CH4, CO2, C2H6, and C2H4 in the vicinity of the critical conditions of water (374 C, 22 MPa). The earlier work has been extended to determine the effect of variations in temperature and feed concentration on the extent of gasification. The percent gasification decreases with increasing feed concentration, indicating an overall kinetic order less than unity. Surprisingly, the percent gasification decreases with increasing temperature. A number of preliminary experiments were conducted with maple sawdust feed, which was thought to be representative of complex organic wastes from paper and vegetable matter. Once again, no solid products were found under the critical conditions; the percent gasification ranged from 16 to 88 percent, depending on the feed composition and residence time.

Modell, M.↗

NASA NTRS1978

Aeronomy of Saturn and Titan

The Saturn system presents exciting and unique objects for planetary aeronomy. The photochemistry of H2 and He leads to the formation of an ionosphere. Methane photolysis results in the formation of spectroscopically detectable amounts of C2H6 and C2H2 and in the case of Titan, C2H4. Density profiles of C2H6, C2H2, and PH3 should be indicative of the strength of atmospheric mixing processes.

Strobel, D. F.↗

NASA NTRS1978

Absolute rate of the reaction of atomic hydrogen with ethylene from 198 to 320 K at high pressure

The rate constant for the H+C2H4 reaction has been measured as a function of temperature. Experiments were performed with high pressures of Ar heat bath gas at seven temperatures from 198 to 320 K with the flash photolysis-resonance fluorescence (FP-RF) technique. Pressures were chosen so as to isolate the addition rate constant k1. The results are well represented by an Arrhenius expression. The results are compared with other studies and are theoretically discussed.

Lee, J. H.↗

NASA NTRS1979

Interstellar synthesis of the cyanopolyynes and related molecules

The cyanopolyynes HC2CN, HC4CN, HC6CN, and HC8CN, and the molecules CH3CHCN and CH3CH2CN, have recently been detected in the interstellar medium. It is shown that the observed abundances of these molecules can be obtained by gas-phase formation pathways if the reaction of H2CN(+) with C2H2 is rapid at low interstellar temperatures. The molecules CH2CHCN and C3N may be formed also by the reactions of H2CN(+) with C2H2, and CH3CH2CN may be formed by reaction of H2CN(+) with C2H4.

Mitchell, G. F.↗

NASA NTRS1979

Optoacoustic detection using Stark modulation

Stark modulation of the absorbed laser radiation in an optoacoustic detector (or spectrophone) is reported. Measurements were made over a range of total pressure between 760 Torr and 50 Torr. Greatly enhanced molecular discrimination is suggested due to the tuning ability of the Stark-shifted absorption. The background signal obtained by operating in this mode is more than 500 times smaller than that obtained by operating the same optoacoustic detector in the conventional chopped radiation mode. The responsivity of the optoacoustic detector and the absorption coefficient of C2H4 are presented as a function of total pressure.

Kavaya, M. J.↗

NASA NTRS1980

Pioneer Venus gas chromatography of the lower atmosphere of Venus

A gas chromatograph mounted in the Pioneer Venus sounder probe measured the chemical composition of the atmosphere of Venus at three altitudes. Ne, N2, O2, Ar, CO, H2O, SO2, and CO2 were measured, and upper limits set for H2, COS, H2S, CH4, Kr, N2O, C2H4, C2H6, and C3H8. Simulation studies have provided indirect evidence for sulfuric acid-like droplets and support the possibility of water vapor at altitudes of 42 and 24 km. The paper discusses the implications of these results for the origin, evolution, and present state of Venus' atmosphere.

Oyama, V. I.↗

NASA NTRS1981

Ethylene in IRC +10216

Ethylene has been detected in the circumstellar gas surrounding the supergiant star IRC +10216. Two lines of the nu sub 7 vibration-rotation band near 28 THz (949/cm) have been seen in absorption at an expansion velocity of 14 km/sec relative to the central star. The line intensities indicate a rotational temperature of T greater than 400 K and a radial C2H4 column density of 10 to the 16th to 10 to the 17th per sq cm.

Betz, A. L.↗

NASA NTRS1981

Atmospheric trace gases - Possibility of sources in the Southern Hemisphere

When measurements of globally distributed trace gases establish their existence in the Southern Hemisphere, it is not always clear whether their presence is due to transport from the Northern Hemisphere or partly from significant sources in the Southern Hemisphere. In this paper a simple criterion is developed whereby one can determine if significant Southern Hemisphere sources exist for a given trace gas. Despite the limitations of the model, there are strong indications that C2 hydrocarbons (C2H2, C2H4, C2H6), CO and CH4 have significant Southern Hemisphere sources.

Khalil, M. A. K.↗

NASA NTRS1981

Remote probing of the atmosphere using a CO2 DIAL system

An overview of our laser remote sensing effort is presented. Using both fundamental and frequency-doubled CO2 laser radiation in a differential absorption LIDAR (DIAL) system, background concentrations of CO, NO, and C2H4 in the atmosphere as well as increases due to localized emission sources have been measured. These species have been detected using the backscattered laser radiation from topographic targets at ranges to 2.7 km with a sensitivity of plus or minus 10 ppb. In addition, using a dual-laser DIAL system, the effect of induced correlation of the LIDAR returns due to atmospheric turbulence has been investigated. These results have been used to help quantify the accuracy of the DIAL measurements and are shown to be consistent with theory.

Killinger, D. K.↗

NASA NTRS1982

Photochemical processes in the inner coma

Models for the inner-coma chemistry of comets are reviewed. The physics relevant to the coma's chemistry is summarized, and the interaction of solar radiation with the coma is described, along with photolytic and chemical processes. The formation and destruction of several observed species are traced through a chemical reaction network, and model results are compared with observations. The species considered include CN, C2, C3, NH2, CH, CO, CO(+), OH, H2O, HCO, C2H4, and C2H3. The models most consistent with observations are shown to indicate that only trace amounts (2% in all) of molecules bearing CN, C2, C3, and NH2 can be present in the nucleus of a comet.

Huebner, W. F.↗

NASA NTRS1983

An analysis of the reflection spectrum of Jupiter from 1500 A to 1740 A

The Jovian reflection spectrum was modeled to determine the mixing ratios of C2H2, the upper limits to mixing ratios of C2H4, C4H2, and NH3, to detect the amount of dust in the stratosphere, and to measure the intensity of the H2 Lyman band dayglow emission. Data were gathered by the IUE spacecraft in the wavelength regions 1500 A to 1740 A, concentrating in the 10 mbar pressure region. Detailed Jupiter model parameters are provided. The mixing ratios of C2H2, C2H6, and C4H2 were found to be near 10 to the -7th, 6.6 x 10 to the -6th, and 2.9 x 10 to the -10th, respectively. Comparisons made with the Voyager 1 and 2 data indicated that the scale height of C2H2 in the 150-10 mbar region is double that of the bulk atmosphere. The data are significant for photochemical modeling of the upper Jovian atmosphere.

Gladstone, G. R.↗