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DOE OSTI2025

Methane pyrolysis by Joule heating for graphitic carbon and hydrogen production

The global energy transition toward sustainability requires technologies that can decarbonize energy carriers and fuels while producing valuable materials. Methane, a primary component of natural gas, is both a high-energy-density fuel and a significant greenhouse gas. This study reports an approach for methane pyrolysis utilizing Joule heating within the deposition substrate to drive the endothermic reaction. With electric current passing through a resistive porous carbon cloth, heat is generated to break C-H bonds of methane molecules. Here, the decomposition of methane as it flows through the cloth results in hydrogen production and the formation of conformally layered graphite around the carbon fibers. The effects of input power, chamber pressure, feedstock flow rate, and process duration on hydrogen and graphite production are characterized via in situ mass spectrometry and laser absorption spectroscopy, resulting in methane conversion rates up to 88%, with hydrogen and carbon yields of 82% and 72%, respectively. Material characterization verifies uniform high-quality graphite deposition, with a Raman I D /I G ratio of 0.1 and 3.38 Å d-spacing. This Joule heating method for catalyst-free methane pyrolysis offers the potential for advancing hydrogen production technology by simultaneously producing valuable materials such as solid graphite, thus enhancing the economic viability of the fuel decarbonization process.

Energy Resources↗
NASA NTRS1974

Pressurant requirements for discharge of liquid methane from a 1.52-meter-(5-ft-) diameter spherical tank under both static and slosh conditions

Pressurized expulsion tests were conducted to determine the effect of various physical parameters on the pressurant gas (methane, helium, hydrogen, and nitrogen) requirements during the expulsion of liquid methane from a 1.52-meter-(5-ft-) diameter spherical tank and to compare results with those predicted by an analytical program. Also studied were the effects on methane, helium, and hydrogen pressurant requirements of various slosh excitation frequencies and amplitudes, both with and without slosh suppressing baffles in the tank. The experimental results when using gaseous methane, helium, and hydrogen show that the predictions of the analytical program agreed well with the actual pressurant requirements for static tank expulsions. The analytical program could not be used for gaseous nitrogen expulsions because of the large quantities of nitrogen which can dissolve in liquid methane. Under slosh conditions, a pronounced increase in gaseous methane requirements was observed relative to results obtained for the static tank expulsions. Slight decreases in the helium and hydrogen requirements were noted under similar test conditions.

Dewitt, R. L.↗
NASA NTRS1974

Bio-conversion of water hyacinths into methane gas, part 1

Bio-gas and methane production from the microbial anaerobic decomposition of water hyacinths (Eichhornia crassipes) (Mart) Solms was investigated. These experiments demonstrated the ability of water hyacinths to produce an average of 13.9 ml of methane gas per gram of wet plant weight. This study revealed that sample preparation had no significant effect on bio-gas and/or methane production. Pollution of water hyacinths by two toxic heavy materials, nickel and cadmium, increased the rate of methane production from 51.8 ml/day for non-contaminated plants incubated at 36 C to 81.0 ml/day for Ni-Cd contaminated plants incubated at the same temperature. The methane content of bio-gas evolved from the anaerobic decomposition of Ni-Cd contaminated plants was 91.1 percent as compared to 69.2 percent methane content of bio-gas collected from the fermentation of non-contaminated plants.

Wolverton, B. C.↗
NASA NTRS1983

Photochemistry of methane in the earth's early atmosphere

The photochemical behavior of methane in the early terrestrial atmosphere is investigated with a detailed model in order to determine how much CH4 might have been present and what types of higher hydroocarbons could have been formed. It is found that any primordial methane accumulated during the course of earth accretion would have been dissipated by photochemical reactions in the atmosphere in a geologically short period of time after the segregation of the core. Abiotic sources of methane are not likely to have been large enough to sustain CH4 mixing ratios as high as 10 to the -6th, the threshold for a possible methane greenhouse, with a CO-rich atmosphere being a possible exception. After the origin of life an increasing biogenic source of methane may have driven CH4 mixing ratios well above 10 to the 6th. The rise of atmospheric oxygen in the early Proterozoic may have led to a more rapid photochemical destruction of methane, lowering the mixing ratio to its present value.

Kasting, J. F.↗
NASA NTRS1983

Interpretation of the 6818.9-A methane feature observed on Jupiter, Saturn, and Uranus

High-resolution (0.1-A) spectra of the 6818.9-A methane feature obtained for Jupiter, Saturn, and Uranus by Baines, Schempp, and Smith (1969) are modeled using a doubling and adding code after Hansen (1983). The feature's rotational quantum number is estimated using the relatively homogeneous atmosphere of Saturn, with only J = 0 and J = 1 fitting the observational constraints. The aerosol content within Saturn's northern temperate region is shown to be substantially less than at the equator, indicating a haze only half as optically thick. Models of Jupiter's atmosphere are consistent with the rotational quantum-number assignment. Synthetic line profiles of the 6818.9-A feature observed on Uranus reveal that a substantial haze exists at or above the methane condensation region with an optical depth eight times greater than previously reported. Seasonal effects are indicated. The methane column abundance is 5 + or - 1 km-am. The mixing ratio of methane to hydrogen within the deep unsaturated region of the planet is 0.045 + or - 0.025, based on an H2 column abundance of 240 + or - 60 km-am (Smith, Macy, and Pilcher /1980/), thus indicating that methane comprises between one-sixth and one-half of the planet's mass. However, proper reevaluation of H2 quadrupole features accounting for the haze reported here may significantly reduce the relative methane abundance.

Baines, K. H.↗
NASA NTRS1984

Atmospheric methane in the recent and ancient atmospheres Concentrations, trends, and interhemispheric gradient

Rasmussen and Khalil (1981) have shown that the concentration of methane is increasing in the earth's atmosphere. A continuing increase of methane may perturb the global environment in the future by warming the earth and leading to more ozone and carbon monoxide in the atmosphere. It appears that the present concentration of methane may be more than twice as high as the natural levels of 150 years ago. An analysis of air bubbles buried long ago in polar ice makes it possible to deduce the concentrations of methane in the old and ancient atmospheres. The present investigation is concerned with the results of an analysis of more than 80 ice core samples, taking into account both polar regions of the earth. The samples range in age from about 100 to nearly 3000 years old. It is found that the concentration of methane started changing significantly about 150 years ago. These findings suggest that the increase of methane is probably indirectly caused by the rapid increase of human population.

Rasmussen, R. A.↗
NASA NTRS1988

Tropospheric methane from an Amazonian floodplain lake

The sources of methane and its flux to the troposphere from the Amazonian floodplain were investigated during the dry season of July and August 1985, using measurements of methane concentration gradients obtained aboard a houseboat laboratory anchored in Lago Calado, a stratified dendritic lake of about 6-sq km area located near the center of the Amazon Basin. Methane concentrations in the mixed layer of the lake were found to vary from 0.0001 to 0.0055 mM, with no consistent temporal trend. The measured methane flux from the surface of the open lake to the atmosphere averaged 27 mg CH4/sq m per day, consistent with the buildup in ambient methane in the nocturnal surface mixed layer of the troposphere. Ebullition contributed 70 percent to the average total flux. The source of methane to the lake and, ultimately, to the troposphere is the benthic sediments.

Crill, Patrick M.↗
NASA NTRS1990

Optical constants of solid methane

Methane is the most abundant simple organic molecule in the outer solar system bodies. In addition to being a gaseous constituent of the atmospheres of the Jovian planets and Titan, it is present in the solid form as a constituent of icy surfaces such as those of Triton and Pluto, and as cloud condensate in the atmospheres of Titan, Uranus, and Neptune. It is expected in the liquid form as a constituent of the ocean of Titan. Cometary ices also contain solid methane. The optical constants for both solid and liquid phases of CH4 for a wide temperature range are needed for radiative transfer calculations, for studies of reflection from surfaces, and for modeling of emission in the far infrared and microwave regions. The astronomically important visual to near infrared measurements of solid methane optical constants are conspicuously absent from the literature. Preliminary results are presented on the optical constants of solid methane for the 0.4 to 2.6 micrometer region. Deposition onto a substrate at 10 K produces glassy (semi-amorphous) material. Annealing this material at approximately 33 K for approximately 1 hour results in a crystalline material as seen by sharper, more structured bands and negligible background extinction due to scattering. The constant k is reported for both the amorphous and the crystalline (annealed) states. Typical values (at absorption maxima) are in the .001 to .0001 range. Below lambda = 1.1 micrometers the bands are too weak to be detected by transmission through the films less than or equal to 215 micrometers in thickness, employed in the studies to date. Using previously measured values of the real part of the refractive index, n, of liquid methane at 110 K, n is computed for solid methane using the Lorentz-Lorenz relationship. Work is in progress to extend the measurements of optical constants n and k for liquid and solid to both shorter and longer wavelengths, eventually providing a complete optical constants database for condensed CH4.

Khare, Bishun N.↗
NASA NTRS1990

Consumption of atmospheric methane by tundra soils

The results of field and laboratory experiments on methane consumption by tundra soils are reported. For methane concentrations ranging from below to well above ambient, moist soils are found to consume methane rapidly; in nonwaterlogged soils, equilibration with atmospheric methane is fast relative to microbial oxidation. It is concluded that lowering of the water table in tundra as a resulting from a warmer, drier climate will decrease methane fluxes and could cause these areas to provide negative feedback for atmospheric methane.

Whalen, S. C.↗
NASA NTRS1989

Optical constants of solid methane

Methane is the most abundant simple organic molecule in the outer solar system bodies. In addition to being a gaseous constituent of the atmospheres of the Jovian planets and Titan, it is present in the solid form as a constituent of icy surfaces such as those of Triton and Pluto, and as cloud condensate in the atmospheres of Titan, Uranus, and Neptune. It is expected in the liquid form as a constituent of the ocean of Titan. Cometary ices also contain solid methane. The optical constants for both solid and liquid phases of CH4 for a wide temperature range are needed for radiative transfer calculations, for studies of reflection from surfaces, and for modeling of emission in the far infrared and microwave regions. The astronomically important visual to near infrared measurements of solid methane optical constants are conspicuously absent from the literature. Preliminary results are presented of the optical constants of solid methane for the 0.4 to 2.6 micron region. K is reported for both the amorphous and the crystalline (annealed) states. Using the previously measured values of the real part of the refractive index, n, of liquid methane at 110 K n is computed for solid methane using the Lorentz-Lorentz relationship. Work is in progress to extend the measurements of optical constants n and k for liquid and solid to both shorter and longer wavelengths, eventually providing a complete optical constants database for condensed CH4.

Khare, Bishun N.↗
NASA NTRS1991

Profiles of alpha 13 C and alpha D in methane from the lower stratosphere

Methane is an important greenhouse gas of biogenic and anthropogenic origin for which global budgets are being constructed from a variety of data. One approach to the global methane budget is the use of the stable isotopes C-13 and D, and the radionuclide C-14 as tracers. The authors measured the isotopic composition of methane from various sources and in tropospheric air for a number of locations. Here, the authors report on the isotopic composition of methane from the lower stratosphere. Measurements of this concentration in the stratosphere can yield estimates for the kinetic isotope effects in the methane destruction reactions. These effects have to be known for quantitative isotopic methane budgets.

Wahlen, Martin↗
NASA NTRS1991

Three-Dimensional Model Synthesis of the Global Methane Cycle

A synthesis of the global methane cycle is presented to attempt to generate an accurate global methane budget. Methane-flux measurements, energy data, and agricultural statistics are merged with databases of land-surface characteristics and anthropogenic activities. The sources and sinks of methane are estimated based on atmospheric methane composition and variations, and a global 3D transport model simulates the corresponding atmospheric responses. The geographic and seasonal variations of candidate budgets are compared with observational data, and the available observations are used to constrain the plausible methane budgets. The preferred budget includes annual destruction rates and annual emissions for various sources. The lack of direct flux measurements in the regions of many of these fluxes makes the unique determination of each term impossible. OH oxidation is found to be the largest single term, although more measurements of this and other terms are recommended.

Fung, I.↗
NASA NTRS1992

Methane transport mechanisms and isotopic fractionation in emergent macrophytes of an Alaskan tundra lake

The stable carbon isotopic composition of methane associated with and emitted by the two dominant emergent macrophytes abundant in the many Alaskan tundra lakes, Carex rostrata and Arctophila fulva, is determined. The carbon isotopic composition of the methane was -58.6 +/- 0.5 (n=2) for Arctophila and -66.6 +/- 2.5 (n=6) for Carex. The methane emitted by these species is depleted in C-13 by 12 per mil for Arctophila and 18 per mil for Carex relative to methane withdrawn from plant stems 1-2 cm below the waterline. The results suggest more rapid transport of (C-12)H4 relative to (C-13)H4 through plants to the atmosphere. Plant stem methane concentrations ranged from 0.2 to 4.0 percent in Arctophila, with an isotopic composition of -46.1 +/- 4.3 percent (n=8). Carex stem methane concentrations ranged from 150 to 1200 ppm, with an isotopic composition of -48.3 +/- 1.4 per mil (n=3).

Chanton, Jeffrey P.↗
NASA NTRS1985

Long term monitoring of methane in the atmosphere by multiplex gas chromatography

Methane is of interest in the study of the Earth's atmosphere because of its implication in the future global warming of the surface. This warming is produced by the absorption of infrared energy by trace gases. It has been estimated that in the next 40 to 50 years, methane could contribute 20 to 25 pct. as much atmospheric warming as that expected from carbon dioxide increases. Studies to examine sources, sinks, and cycles of methane will require analytical methods capable of continuous unattended measurement with temporal resolution of an hour or less for weeks at a time. Gas chromatography (GC) is one of the most practical methods available to conduct the analysis of air, but limitations in this technique still exist which can be alleviated with multiplex GC (MGC). MGC is a technique where many samples are pseudo-randomly introduced to the chromatograph without regard to the length of time required for an analysis. The resulting data must then be reduced using computational methods such as cross correlation. In the technique reported, a tube packed with silver oxide was used at the inlet of the GC column to create concentration pulses of methane in a sample stream of air. By using only one carrier, i.e., ambient air, an effective and accurate method to monitor the variations in concentration of methane in the atmosphere over long periods of time was developed. Methane in ambient air was monitored for an eight day period and an interesting temporal variability was found. This work has shown the utility of a relatively simple MGC for the analysis of a real environmental sample.

Valentin, Jose R.↗
NASA NTRS1994

Mars methane engine

The feasibility of an internal combustion engine operating on a mixture of methane, carbon dioxide, and oxygen has been verified by previous design groups for the Mars Methane Engine Project. Preliminary stoichiometric calculations examined the theoretical fuel-air ratios needed for the combustion of methane. Installation of a computer data acquisition system along with various ancillary components will enable the performance of the engine, running on the described methane mixture, to be optimized with respect to minimizing excess fuel. Theoretical calculations for stoichiometric combustion of methane-oxygen-carbon dioxide mixtures yielded a ratio of 1:2:4.79 for a methane-oxygen-carbon dioxide mixture. Empirical data shows the values to be closer to 1:2.33:3.69 for optimum operation.

Bui, Hung↗
NASA NTRS1994

Eddy correlation measurements of methane fluxes using a tunable diode laser at the Kinosheo Lake tower site during the Northern Wetlands Study (NOWES)

As part of the Canadian Northern Wetlands Study (NOWES) measurements of methane flux were made at the Kinosheo Lake tower site for a 1-month period during the 1990 summer intensive. The measurements were made with a diode-laser-based methane sensor using the eddy correlation technique. Measurements of the methane fluxes were made at two levels, 5 or 18 m. Approximately 900 half-hour average methane flux measurements were obtained. Weak temporal and diurnal trends were observed in the data. Fluxes averaged over the study period showed an overall methane emission of 16 mg CH4 m(exp -2)/d with a daytime average of 20 mg CH4 m(exp -2)/d and a nighttime average of 9 mg CH4 m(exp -2)/d. The effect of emission footprint was evident in the data. A strong relationship between the daily average methane flux and wet bog temperature at 20-cm depth was observed.

Edwards, G. C.↗
NASA NTRS2000

Photochemistry of Methane in Model Atmospheres of Jupiter and Titan

The two central findings were 1) hydrogen atoms and hydrogen molecules photodissociated from methane are relatively richer in H than in D in other words deuterium atoms have a greater probability of remaining attached to the carbon atom. Titan, a moon of Saturn has an atmosphere which is largely nitrogen but also contains about 3% methane as well as smaller amounts of C2 and C3 hydrocarbons. If all these hydrocarbons are of biological origin, the isotopic scrambling occurring in living organisms would result in equal D atom abundances. On the other hand, if the higher hydrocarbons are derived from methane by photodissociation of methane, they should be richer in D than methane. Precise values for the enrichment were derived from our photochemical data. 2) When methane is dissociated by vuv light, methylene is produced in a singlet state. This explains why the higher hydrocarbons are sparse on Jupiter but relatively rich on Titan.

Bersohn, Richard↗
NASA NTRS1982

Methane-Powered Vehicles

Liquid methane is beginning to become an energy alternative to expensive oil as a power source for automotive vehicles. Methane is the principal component of natural gas, costs less than half as much as gasoline, and its emissions are a lot cleaner than from gasoline or diesel engines. Beech Aircraft Corporation's Boulder Division has designed and is producing a system for converting cars and trucks to liquid methane operation. Liquid methane (LM) is a cryogenic fuel which must be stored at a temperature of 260 degrees below zero Fahrenheit. The LM system includes an 18 gallon fuel tank in the trunk and simple "under the hood" carburetor conversion equipment. Optional twin-fuel system allows operator to use either LM or gasoline fuel. Boulder Division has started deliveries for 25 vehicle conversions and is furnishing a liquid methane refueling station. Beech is providing instruction for Northwest Natural Gas, for conversion of methane to liquid state.

Source record↗