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NASA NTRS2009

C-12/C-13 Ratio in Ethane on Titan and Implications for Methane's Replenishment

The C-12/C-13 abundance ratio in ethane in the atmosphere of Titan has been measured at 822 cm(sup -1) from high spectral resolution ground-based observations. The value 89(8), coincides with the telluric standard and also agrees with the ratio seen in the outer planets. It is almost identical to the result for ethane on Titan found by the composite infrared spectrometer (CIRS) on Cassini. The C-12/C-13 ratio for ethane is higher than the ratio measured in atmospheric methane by Cassini/Huygens GCMS, 82.3(l), representing an enrichment of C-12 in the ethane that might be explained by a kinetic isotope effect of approximately 1.1 in the formation of methyl radicals. If methane is being continuously resupplied to balance photochemical destruction, then we expect the isotopic composition in the ethane product to equilibrate at close to the same C-12/C-13 ratio as that in the supply. The telluric value of the ratio in ethane then implies that the methane reservoir is primordial.

Jennings, Donald E.↗

NASA NTRS2004

Fuels Containing Methane of Natural Gas in Solution

While exploring ways of producing better fuels for propulsion of a spacecraft on the Mars sample return mission, a researcher at Johnson Space Center (JSC) devised a way of blending fuel by combining methane or natural gas with a second fuel to produce a fuel that can be maintained in liquid form at ambient temperature and under moderate pressure. The use of such a blended fuel would be a departure for both spacecraft engines and terrestrial internal combustion engines. For spacecraft, it would enable reduction of weights on long flights. For the automotive industry on Earth, such a fuel could be easily distributed and could be a less expensive, more efficient, and cleaner-burning alternative to conventional fossil fuels. The concept of blending fuels is not new: for example, the production of gasoline includes the addition of liquid octane enhancers. For the future, it has been commonly suggested to substitute methane or compressed natural gas for octane-enhanced gasoline as a fuel for internal-combustion engines. Unfortunately, methane or natural gas must be stored either as a compressed gas (if kept at ambient temperature) or as a cryogenic liquid. The ranges of automobiles would be reduced from their present values because of limitations on the capacities for storage of these fuels. Moreover, technical challenges are posed by the need to develop equipment to handle these fuels and, especially, to fill tanks acceptably rapidly. The JSC alternative to provide a blended fuel that can be maintained in liquid form at moderate pressure at ambient temperature has not been previously tried. A blended automotive fuel according to this approach would be made by dissolving natural gas in gasoline. The autogenous pressure of this fuel would eliminate the need for a vehicle fuel pump, but a pressure and/or flow regulator would be needed to moderate the effects of temperature and to respond to changing engine power demands. Because the fuel would flash as it entered engine cylinders, relative to gasoline, it would disperse more readily and therefore would mix with air more nearly completely. As a consequence, this fuel would burn more nearly completely (and, hence, more cleanly) than gasoline does. The storage density of this fuel would be similar to that of gasoline, but its energy density would be such that the mileage (more precisely, the distance traveled per unit volume of fuel) would be greater than that of either gasoline or compressed natural gas. Because the pressure needed to maintain the fuel in liquid form would be more nearly constant and generally lower than that needed to maintain compressed natural gas in liquid form, the pressure rating of a tank used to hold this fuel could be lower than that of a tank used to hold compressed natural gas. A mixture of natural gas and gasoline could be distributed more easily than could some alternative fuels. A massive investment in new equipment would not be necessary: One could utilize the present fuel-distribution infrastructure and could blend the gasoline and natural gas at almost any place in the production or distribution process - perhaps even at the retail fuel pump. Yet another advantage afforded by use of a blend of gasoline and natural gas would be a reduction in the amount of gasoline consumed. Because natural gas costs less than gasoline does and is in abundant supply in the United States, the cost of automotive fuel and the demand for imported oil could be reduced.

Sullivan, Thomas A.↗

NASA NTRS2012

Titan's Tropopause Temperatures from CIRS: Implications for Stratospheric Methane Cloud Formation

Analysis of Cassini Composite Infrared Spectrometer (CIRS) far-IR spectra enable the construction of Titan's temperature profile in the altitude region containing the tropopause. Whereas the methane V4 band at 1306/cm (7.7 microns) is the primary opacity source for deducing thermal structure between 100 km and 500 km, N2-N2 collision-induced absorption between 70 and 140/cm (143 microns and 71 microns) is utilized to determine temperatures at Titan's tropopause. Additional opacity due to aerosol and nitrile ices must also be taken into account in this part of the far-IR spectral region. The spectral characteristics of these particulate opacities have been deduced from CIRS limb data at 58degS, 15degS, 15degN, and 85degN. Empirically, the spectral shapes of these opacities appear to be independent of both latitude and altitude below 300 km (Anderson and Samuelson, 2011, Icarus 212, 762-778), justifying the extension of these spectral properties to all latitudes. We find that Titan's tropopause temperature is cooler than the HAS! value of 70.5K by approx. 6K. This leads to the possibility that subsidence at high northern latitudes can cause methane condensation in the winter polar stratosphere. A search for methane clouds in this region is in progress.

Anderson, C. M.↗

NASA NTRS2010

Creating Methane from Plastics: Recycling at a Lunar Outpost

The high cost of re-supply from Earth demands resources to be utilized to the fullest extent for exploration missions. Recycling is a key technology that maximizes the available resources by converting waste products into useful commodities. One example of this is to convert crew member waste such as plastic packaging, food scraps, and human waste, into fuel. The ability to refuel on the lunar surface would reduce the vehicle mass during launch and provide excess payload capability. The goal of this project is to determine the feasibility of recycling waste into methane on the lunar outpost by performing engineering assessments and lab demonstrations of the technology. The first goal of the project was to determine how recycling could influence lunar exploration. Table I shows an estimation of the typical dried waste stream generated each day for a crew of four. Packaging waste accounts for nearly 86% of the dry waste stream and is a significant source of carbon on the lunar surface. This is important because methane (CH4) can be used as fuel and no other source of carbon is available on the lunar surface. With the initial assessment indicating there is sufficient resources in the waste stream to provide refueling capabilities, the project was designed to examine the conversion of plastics into methane.

Captain, Janine↗

NASA NTRS2012

Global Air Quality and Health Co-benefits of Mitigating Near-term Climate Change Through Methane and Black Carbon Emission Controls

Tropospheric ozone and black carbon (BC), a component of fine particulate matter (PM < or = 2.5 microns in aerodynamic diameter; PM2.5), are associated with premature mortality and they disrupt global and regional climate. Objectives: We examined the air quality and health benefits of 14 specific emission control measures targeting BC and methane, an ozone precursor, that were selected because of their potential to reduce the rate of climate change over the next 20-40 years. Methods: We simulated the impacts of mitigation measures on outdoor concentrations of PM2.5 and ozone using two composition-climate models, and calculated associated changes in premature PM2.5‑ and ozone-related deaths using epidemiologically derived concentration-response functions. Results: We estimated that, for PM2.5 and ozone, respectively, fully implementing these measures could reduce global population-weighted average surface concentrations by 23-34% and 7-17% and avoid 0.6-4.4 and 0.04-0.52 million annual premature deaths globally in 2030. More than 80% of the health benefits are estimated to occur in Asia. We estimated that BC mitigation measures would achieve approximately 98% of the deaths that would be avoided if all BC and methane mitigation measures were implemented, due to reduced BC and associated reductions of nonmethane ozone precursor and organic carbon emissions as well as stronger mortality relationships for PM2.5 relative to ozone. Although subject to large uncertainty, these estimates and conclusions are not strongly dependent on assumptions for the concentration-response function. Conclusions: In addition to climate benefits, our findings indicate that the methane and BC emission control measures would have substantial co-benefits for air quality and public health worldwide, potentially reversing trends of increasing air pollution concentrations and mortality in Africa and South, West, and Central Asia. These projected benefits are independent of carbon dioxide mitigation measures. Benefits of BC measures are underestimated because we did not account for benefits from reduced indoor exposures and because outdoor exposure estimates were limited by model spatial resolution.

air quality↗

NASA NTRS2016

Foundational Methane Propulsion Related Technology Efforts, and Challenges for Applications to Human Exploration Beyond Earth Orbit

Current interest in human exploration beyond earth orbit is driving requirements for high performance, long duration space transportation capabilities. Continued advancement in photovoltaic power systems and investments in high performance electric propulsion promise to enable solar electric options for cargo delivery and pre-deployment of operational architecture elements. However, higher thrust options are required for human in-space transportation as well as planetary descent and ascent functions. While high thrust requirements for interplanetary transportation may be provided by chemical or nuclear thermal propulsion systems, planetary descent and ascent systems are limited to chemical solutions due to their higher thrust to weight and potential planetary protection concerns. Liquid hydrogen fueled systems provide high specific impulse, but pose challenges due to low propellant density and the thermal issues of long term propellant storage. Liquid methane fueled propulsion is a promising compromise with lower specific impulse, higher bulk propellant density and compatibility with proposed in-situ propellant production concepts. Additionally, some architecture studies have identified the potential for commonality between interplanetary and descent/ascent propulsion solutions using liquid methane (LCH4) and liquid oxygen (LOX) propellants. These commonalities may lead to reduced overall development costs and more affordable exploration architectures. With this increased interest, it is critical to understand the current state of LOX/LCH4 propulsion technology and the remaining challenges to its application to beyond earth orbit human exploration. This paper provides a survey of NASA's past and current methane propulsion related technology efforts, assesses the accomplishments to date, and examines the remaining risks associated with full scale development.

Brown, Thomas↗

NASA NTRS2016

Airborne Measurements of Atmospheric Methane Using Pulsed Laser Transmitters

Atmospheric methane (CH4) is the second most important anthropogenic greenhouse gas with approximately 25 times the radiative forcing of carbon dioxide (CO2) per molecule. At NASA Goddard Space Flight Center (GSFC) we have been developing a laser-based technology needed to remotely measure CH4 from orbit. We report on our development effort for the methane lidar, especially on our laser transmitters and recent airborne demonstration. Our lidar transmitter is based on an optical parametric process to generate near infrared laser radiation at 1651 nanometers, coincident with a CH4 absorption. In an airborne flight campaign in the fall of 2015, we tested two kinds of laser transmitters --- an optical parametric amplifier (OPA) and an optical parametric oscillator (OPO). The output wavelength of the lasers was rapidly tuned over the CH4 absorption by tuning the seed laser to sample the CH4 absorption line at several wavelengths. This approach uses the same Integrated Path Differential Absorption (IPDA) technique we have used for our CO2 lidar for ASCENDS. The two laser transmitters were successfully operated in the NASAs DC-8 aircraft, measuring methane from 3 to 13 kilometers with high precision.

optical radar↗

NASA NTRS2016

Developing Atmospheric Retrieval Methods for Direct Imaging Spectroscopy of Gas Giants in Reflected Light I: Methane Abundances and Basic Cloud Properties

Reflected light spectroscopy and photometry of cool, directly imaged extrasolar giant planets are expected to be performed in the next decade by space-based telescopes equipped with optical wavelength coronagraphs and integral field spectrographs, such as the Wide-Field Infrared Survey Telescope (WFIRST). We are developing a new atmospheric retrieval methodology to help assess the science return and inform the instrument design for such future missions, and ultimately interpret the resulting observations. Our retrieval technique employs an albedo model coupled with both a Markov chain Monte Carlo Ensemble Sampler (emcee) and a multimodal nested sampling algorithm (MultiNest) to map the posterior distribution. This combination makes the global evidence calculation more robust for any given model, and highlights possible discrepancies in the likelihood maps. Here we apply this methodology to simulated spectra of cool giant planets. As a proof-of-concept, our current atmospheric model contains 1 or 2 cloud layers, methane as a major absorber, and a H2-He background gas. This 6-to-9 parameter model is appropriate for Jupiter-like planets and can be easily expanded in the future. In addition to deriving the marginal likelihood distribution and confidence intervals for the model parameters, we perform model selection to determine the significance of methane and cloud detection as a function of expected signal-to-noise, in the presence of spectral noise correlations. After internal validation, the method is applied to realistic reflected-light spectra of Jupiter, Saturn, and HD 99492 c, a likely observing target. We find that the presence or absence of clouds and methane can be determined with high accuracy, while parameters uncertainties are model-dependent.

spectroscopy↗

NASA NTRS2018

Experimental Effervescence and Freezing Point Depression Measurements of Nitrogen in Liquid Methane-Ethane Mixtures

NASA is designing an unmanned submarine to explore the depths of the hydrocarbon-rich seas on Saturn's moon Titan. Data from Cassini indicates that the Titan north polar environment sustains stable seas of variable concentrations of ethane, methane, and nitrogen, with a surface temperature near 93 K. The submarine must operate autonomously, study atmosphere/sea exchange, interact with the seabed, hover at the surface or any depth within the sea, and be capable of tolerating variable hydrocarbon compositions. Currently, the main thermal design concern is the effect of effervescence on submarine operation, which affects the ballast system, science instruments, and propellers. Twelve effervescence measurements on various liquid methane-ethane compositions with dissolved gaseous nitrogen are thus presented from 1.5 bar to 4.5 bar at temperatures from 92 K to 96 K to simulate the conditions of the seas. After conducting effervescence measurements, two freezing point depression measurements were conducted. The freezing liquid line was depressed more than 15 K below the triple point temperatures of pure ethane (90.4 K) and pure methane (90.7 K). Experimental effervescence measurements will be used to compare directly with effervescence modeling to determine if changes are required in the design of the thermal management system as well as the propellers.

Submarine↗

NASA NTRS2019

Hydrogen Recovery by Methane Pyrolysis to Elemental Carbon

Use of a Sabatier reactor to recover the oxygen from the carbon dioxide exhaled by the crew on the International Space Station has been limited by the loss of the hydrogen contained in the methane it generates. Maximizing the oxygen recovered requires the hydrogen to be recovered from the methane product and recycled back to the Sabatier reactor. We describe the use of a tailored methane pyrolysis reactor to completely recover this hydrogen. The carbon-containing byproduct is elemental carbon, which is generated in the form of easily handled, non-sooty material that may have various uses. The process of creating this tailored carbon vapor deposition process involved exploration of the effects of temperature, pressure, substrate design and other variables to develop a high yield process that cleanly generates the desired products. Reaction kinetics and kinetics modelling were used to specify the temperature, pressure and reactor volume required to achieve the target conversion and to assure that the final average density was as high as possible. Reactor design included the selection of materials that will survive the high temperatures and environment in the pyrolysis reactor, and thermal modeling to achieve the required temperatures with minimum power consumption. The successful construction and demonstration of a brassboard prototype will allow the results of the chemical, thermal and mechanical models to be validated and should provide a useful alternative for a completely closed loop ECLS system. Integration of this technology with state-of-the-art (SOA) Sabatier hardware on ISS requires a complete understanding of the effects of impurities in the product hydrogen on the Sabatier catalyst. SOA Sabatier catalyst was evaluated over short and long-term exposure to anticipated contaminants to identify effects.

Yates, Stephen F.↗

NASA NTRS2019

Hydrogen Recovery by Methane Pyrolysis to Elemental Carbon

Yates, Stephen F.↗

NASA NTRS2022

Recommended Direct Simulation Monte Carlo Collision Model Parameters for Reacting Methane Flows

While hydrocarbon combustion and gas-surface interactions have been simulated for a variety of applications in continuum solvers, such processes have been rarely investigated in Direct Simulation Monte Carlo (DSMC). Thus Variable Hard/Soft Sphere (VHS/VSS)collision parameters are not available for most molecules of interest in the decomposition of methane, a significant pyrolysis gas product and potential atmospheric species for Titan re-entries. As these properties are essential for accurate modeling of gas transport and thermochemical effects, a method must be devised to compute them for use in DSMC. In this study, the methodology outlined in Stephani et al is utilized to compute the VHS/VSS parameters by fitting the Ω(1,1)and Ω(2,2) collision integrals [1]. These collision integrals are typically computed from intermolecular potentials and are used in CFD simulations to calculate transport properties such as viscosity, thermal conductivity, and diffusion. This approach ensures consistency between micro-scale collisions and macro-scale transport properties. To produce the necessary collision integrals needed for the fitting routine, we utilize the method described by Laricchiuta et al, where collision integrals are computed based on the constituent particles’ polarizability and effective electron number [2].Preliminary computations of pure-species Ω(1,1)and Ω(2,2)collision integrals produced from the coupled approach of Stephani et al and Laricchiuta et al for methane show good agreement with those computed via available ab-initio Potential Energy Surface Computations, as seen in Figure 1. Above 300K, no more than 12% deviation is observed between the two results over the temperature range of the fitted PES data [3].Current results of this study include full collision-specificVSS transport properties for a complex-species mixture involving major byproducts of pure methane decomposition. Targeted final results will include a comprehensive list of VSS parameters relevant toDSMC simulations of Titan atmospheric entry, based on the reduced kinetic model of Savajano et al [4].

M R Gosma↗

NASA NTRS2022

Methane Bioreactor System Offers Sustainable Plastic Alternative for Earth and Space

Mango Materials partnered with the Colorado School of Mines on NASA STTR awards to adapt a bioreactor system to convert methane into bioplastic for low-gravity environments. In space, methane from carbon dioxide conversion systems and waste treatment can be used to 3D print objects and provide polymers for construction and regolith binding. On Earth, the system can convert methane—a greenhouse gas—into environmentally conscious bioplastic. Mango Materials received $6 million through NASA CCRPP, including funds from fashion investors seeking alternatives to plastic-based textiles.

SBIR/STTR↗

NASA NTRSDate not supplied

Computational Fluid Dynamics Simulation of Methane Slosh and Drain Experiments

NASA possesses a wealth of historical cryogenic experiments that provide valuable insights into the design, troubleshooting, and understanding involved in the complex fluid and thermodynamics of managing cryogenic propellants. One approach to leveraging these historical datasets is by simulating these experiments to validate the accuracy of simulation environments and constituent models. This study focused on simulating a selection of the K site test series for both static and sloshing pressurized liquid methane draining experiments conducted at NASA in the 1970’s, utilizing computational fluid dynamics. The simulations were performed in the ANSYS FLUENT environment using the Volume of Fluid (VOF) numerical approach. A k-omega turbulence model was used with interfacial turbulence damping, and accurately predicted the amount of pressurant needed to maintain the required tank pressure throughout the static drain. The static simulation predicted the temperature stratification in the ullage observed at the end of the drain. During the methane expulsion with sloshing test, many features were successfully captured using the k-omega turbulence model with interfacial turbulence damping included. The rate of phase change and liquid temperature was overpredicted compared to the experimental measurements. The overprediction may be attributed to uncertainties in the vessel geometry, methane pressurant temperature and composition, and methodological differences in how the sloshing frequency was adjusted during the expulsion.

Cryogenic Propellants↗

DOE OSTI2024

Synthesis and oxidation of methane

The present disclosure describes genes and proteins of the coenzyme F430 synthetic pathway. The genes and proteins in the pathway find uses as isolated nucleic acids, transformation vectors, a transformation media, genetically modified cells, methods of modulating methanogenesis, methods of modulating methane oxidation, methods of making a tetrapyrrole compound, methods of oxidizing methane, methods of biogenic methane synthesis is provided, methods of assaying an organism for potential methanogenic or methanotrophic activity, and isolated proteins.

Mansoorabadi, Steven↗

DOE OSTI2024

Simulated plant-mediated oxygen input has strong impacts on fine-scale porewater biogeochemistry and weak impacts on integrated methane fluxes in coastal wetlands

Methane (CH 4 ) emissions from wetland ecosystems are controlled by redox conditions in the soil, which are currently underrepresented in Earth system models. Plant-mediated radial oxygen loss (ROL) can increase soil O 2 availability, affect local redox conditions, and cause heterogeneous distribution of redox-sensitive chemical species at the root scale, which would affect CH 4 emissions integrated over larger scales. In this study, we used a subsurface geochemical simulator (PFLOTRAN) to quantify the effects of incorporating either spatially homogeneous ROL or more complex heterogeneous ROL on model predictions of porewater solute concentration depth profiles (dissolved organic carbon, methane, sulfate, sulfide) and column integrated CH 4 fluxes for a tidal coastal wetland. From the heterogeneous ROL simulation, we obtained 18% higher column averaged CH 4 concentration at the rooting zone but 5% lower total CH 4 flux compared to simulations of the homogeneous ROL or without ROL. This difference is because lower CH 4 concentrations occurred in the same rhizosphere volume that was directly connected with plant-mediated transport of CH 4 from the rooting zone to the atmosphere. Sensitivity analysis indicated that the impacts of heterogeneous ROL on model predictions of porewater oxygen and sulfide concentrations will be more important under conditions of higher ROL fluxes or more heterogeneous root distribution (lower root densities). Despite the small impact on predicted CH 4 emissions, the simulated ROL drastically reduced porewater concentrations of sulfide, an effective phytotoxin, indicating that incorporating ROL combined with sulfur cycling into ecosystem models could potentially improve predictions of plant productivity in coastal wetland ecosystems.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

A review on advances in oxidative coupling of methane (OCM) for industrial use and prospects of CO 2 –H 2 O splitting integration

The discovery of shale gas reserves has encouraged the development of direct methods for methane conversion into valuable chemicals, offering an alternative to indirect approaches that involve an energy-intensive and intermittent syngas production step, leading to high CO 2 emissions. Amongst the direct methods, the oxidative coupling of methane (OCM) is a potential pathway to reduce CO 2 emissions and can produce commodity chemicals such as ethylene, a chemical regarded as central to the petrochemical industry. Even though OCM has been studied for over four decades, the technology still has not found commercial application. Amongst the challenges regarding industrial deployment of OCM, the most significant one is the requirement of a high ethylene yield of 30 % which is currently reported to be around 20 %. Moreover, the highly exothermic nature of the process and controlling the carbon selectivity over oxides of carbon (COx) is the heart of the problem. Numerous researchers have presented promising results in terms of catalysts, reactor designs and feeding strategies for OCM. However, due to lack of inclusiveness in the results, none of the combination of catalysts, reactors and system optimizations has been able to bring about its industrial viability. The current paper presents an extensive review of the noteworthy attempts to achieve industrial targets for OCM. Moreover, a comprehensive criteria is presented which highlights the desired end state for the industrial deployment of OCM technology. Furthermore, the criteria is based on literature survey and a comparison with industrially deployed ethylene production plants i.e., naphtha or ethane steam cracker plants. Finally, a novel integration technology is presented which includes a combination of OCM and CO 2 -H 2 O splitting in a chemical looping reactor design to enable efficient energy utilization and minimal heat losses to the environment.

CO2 Splitting↗

DOE OSTI2026

MoS 2 Catalysts Selectively Achieve High Yield of Liquid Oxygenate from Direct Conversion of Methane via Hydroxyl Radicals

Directly converting methane (CH 4 ) into liquid oxygenates (e.g., methanol) can circumvent the cost and engineering limits of natural gas transportation and storage. However, oxygenate yields from CH 4 remain low, and sulfur present in natural gas hinders activity in most catalysts. Here, to overcome these barriers, we employ bulk molybdenum disulfide (MoS 2 ), a low-cost, robust catalyst which selectively produces large quantities of liquid oxygenates (>900 µmol/g cat ∙hr) from methane in the presence of hydroxyl (OH • ) radicals produced from dilute hydrogen peroxide (H 2 O 2 ) at 75°C. Under realistic reaction conditions, MoS 2 partially and reversibly adopts a metastable, more electrically conductive phase (1T’) that can only be observed through in situ structural probes. Herein, we elucidate that redox synergy between H 2 O 2 and MoS 2 produces active OH • radical species that selectively transform CH 4 to surface methoxy species at the gas-solid liquid interface, leading to the unitary production of liquid oxygenate at a rate competitive with more costly precious metal catalysts, without additional catalyst preparation steps.

36 MATERIALS SCIENCE↗