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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 NTRS1990

Nuclear thermal rockets using indigenous extraterrestrial propellants

A preliminary examination of a concept for a Mars and outer solar system exploratory vehicle is presented. Propulsion is provided by utilizing a nuclear thermal reactor to heat a propellant volatile indigenous to the destination world to form a high thrust rocket exhaust. Candidate propellants, whose performance, materials compatibility, and ease of acquisition are examined and include carbon dioxide, water, methane, nitrogen, carbon monoxide, and argon. Ballistics and winged supersonic configurations are discussed. It is shown that the use of this method of propulsion potentially offers high payoff to a manned Mars mission. This is accomplished by sharply reducing the initial mission mass required in low earth orbit, and by providing Mars explorers with greatly enhanced mobility in traveling about the planet through the use of a vehicle that can refuel itself each time it lands. Thus, the nuclear landing craft is utilized in combination with a hydrogen-fueled nuclear-thermal interplanetary launch. By utilizing such a system in the outer solar system, a low level aerial reconnaissance of Titan combined with a multiple sample return from nearly every satellite of Saturn can be accomplished in a single launch of a Titan 4 or the Space Transportation System (STS). Similarly a multiple sample return from Callisto, Ganymede, and Europa can also be accomplished in one launch of a Titan 4 or the STS.

Zubrin, Robert M.↗

NASA NTRS2017

Vehicle-Level Oxygen/Methane Propulsion System Hotfire Testing at Thermal Vacuum Conditions

A prototype integrated liquid oxygen/liquid methane propulsion system was hot-fire tested at a variety of simulated altitude and thermal conditions in the NASA Glenn Research Center Plum Brook Station In-Space Propulsion Thermal Vacuum Chamber (formerly B2). This test campaign served two purposes: 1) Characterize the performance of the Plum Brook facility in vacuum accumulator mode and 2) Collect the unique data set of an integrated LOX/Methane propulsion system operating in high altitude and thermal vacuum environments (a first). Data from this propulsion system prototype could inform the design of future spacecraft in-space propulsion systems, including landers. The test vehicle for this campaign was the Integrated Cryogenic Propulsion Test Article (ICPTA), which was constructed for this project using assets from the former Morpheus Project rebuilt and outfitted with additional new hardware. The ICPTA utilizes one 2,800 lbf main engine, two 28 lbf and two 7 lbf reaction control engines mounted in two pods, four 48-inch propellant tanks (two each for liquid oxygen and liquid methane), and a cold helium system for propellant tank pressurization. Several hundred sensors on the ICPTA and many more in the test cell collected data to characterize the operation of the vehicle and facility. Multiple notable experiments were performed during this test campaign, many for the first time, including pressure-fed cryogenic reaction control system characterization over a wide range of conditions, coil-on-plug ignition system demonstration at the vehicle level, integrated main engine/RCS operation, and a non-intrusive propellant mass gauging system. The test data includes water-hammer and thermal heat leak data critical to validating models for use in future vehicle design activities. This successful test campaign demonstrated the performance of the updated Plum Brook In-Space Propulsion thermal vacuum chamber and incrementally advanced the state of LOX/Methane propulsion technology through numerous system-level and subsystem experiments.

Morehead, Robert L.↗

DOE OSTI2025

Technoeconomic Analysis of Microwave-Assisted Dry Reforming Integrated with Chemical Looping for Production of Methanol

Methanol is a key component in producing formaldehyde, acetic acid, and methyl tert -butyl ether (MTBE) and supports a wide array of industries, including plastics, textiles, and automotive. It also plays a growing role in renewable energy solutions. However, the conventional production of methanol involves steam reforming of methane, which is very energy-intensive and produces significant quantities of the greenhouse gas carbon dioxide. In this research, a chemical looping scheme is combined with dry reforming of natural gas in a novel microwave reactor to produce an industrial quantity of methanol. A heat exchanger network is developed to substantially reduce hot and cold utility usage. The effect of the cost of purchasing carbon dioxide from an external source for dry reforming, the capital cost of the microwave reactor, and the cost of electricity on the net present value is analyzed. Technoeconomic comparison with the conventional industrial process that produces methanol via steam reforming of methane indicates that the chemical looping generates a significant positive net present value along with a substantial reduction in carbon dioxide emissions while producing methanol significantly below the U.S. Department of Energy’s goal of $800/ton.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Assessing the Relative Climate Impact of Carbon Utilization for Concrete, Chemical, and Mineral Production

Estimates show that 6.2 gigatons of carbon dioxide (CO2) can be captured and utilized across three pathways, concrete, chemical, and minerals, by 2050. However, it is difficult to compare the climate benefit across these three carbon capture and utilization (CCU) pathways to determine the most effective use of captured CO2. The life cycle assessment methods to evaluate the climate benefit of CCU chemicals should additionally account for the change in material properties of concrete due to CO2 utilization. Furthermore, with most CO2 utilization technologies being in the early stages of research and development, the uncertainty and variability in process and inventory data present a significant challenge in evaluating the climate benefit. We present a stochastically determined climate return on investment (ROI) metric to rank and prioritize CO2 utilization across 20 concrete, chemical and mineral pathways based on the realized climate benefit. We show that two concrete pathways, which use CO2 during concrete mixing, and two chemical pathways, which produce formic acid through hydrogenation of CO2 and carbon monoxide through dry reforming of methane, generate the greatest climate ROI and are the only CCU pathways with a higher likelihood of generating a climate benefit than a climate burden.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2022

Can CO 2 -assisted alkane dehydrogenation lead to negative CO 2 emissions?

The utilization of light alkanes to generate value-added chemicals has gained significant attention due to the U.S. shale gas boom in recent decades. For example, after methane, ethane (3-16 vol.%) and propane (up to 5 vol.%) are the most abundant hydrocarbon species in shale gas deposits. Further, these inexpensive, widely available, but often underutilized, light alkanes can be used as a feedstock to produce olefins, which are among the most important petrochemical building blocks in chemical industry. Ethylene and propylene are used in the production of polymers (e.g., polyethylene, polypropylene) and epoxides (e.g., ethylene oxide, propylene oxide), as well as intermediates in the manufacture of numerous other chemicals (e.g., ethylene glycol, ethylbenzene, acetone, isopropanol, acrylonitrile).

03 NATURAL GAS↗

NASA NTRS1986

Recent concepts in missions to Mars - Extraterrestrial processes

This paper presents some recent concepts in Mars Sample Return (MSR) missions that utilize extraterrestrial resources. The concepts examined include the power and energy needs of this mission. It is shown that solar energy is not especially attractive. Radioisotopic power generator and a Rankine cycle use are seen to be viable options. Quantitative estimates, taking into consideration state-of-the-art and projected technologies indicate that the power/energy per se is not critical to the mission - but reliability is. Hence, various modern options for the components of the power generation and utilization are discussed. The dramatic savings in Shuttle (or other) vehicle launches are quantitatively plotted. The basic system that is discussed here is the production of hydrocarbon (methane) fuel and oxygen from Martian atmosphere. For the simplest mission, it is seen that earth-carried methane burned with oxygen produced on site provides the best system.

Ramohalli, K. N.↗

NASA NTRS2001

A Survey of Alternative Oxygen Production Technologies

Utilization of the Martian atmosphere for the production of fuel and oxygen has been extensively studied. The baseline fuel production process is a Sabatier reactor, which produces methane and water from carbon dioxide and hydrogen. The oxygen produced from the electrolysis of the water is only half of that needed for methane-based rocket propellant, and additional oxygen is needed for breathing air, fuel cells and other energy sources. Zirconia electrolysis cells for the direct reduction of CO2 arc being developed as an alternative means of producing oxygen, but present many challenges for a large-scale oxygen production system. The very high operating temperatures and fragile nature of the cells coupled with fairly high operating voltages leave room for improvement. This paper will survey alternative oxygen production technologies, present data on operating characteristics, materials of construction, and some preliminary laboratory results on attempts to implement each. Our goal is to significantly improve upon the characteristics of proposed zirconia cells for oxygen production. To achieve that goal we are looking at electrolytic systems that operate at significantly lower temperatures, preferably below 31C to allow the incorporation of liquid CO2 in the electrolyte. Our preliminary results indicate that such a system will have much higher current densities and have simpler cathode construction than a porous gas feed electrode system. Such a system could be achieved based on nonaqueous electrolytes or ionic liquids. We are focusing our research on the anode reaction that will produce oxygen from a product generated at the cathode using CO2 as the feed. Operation at low temperatures also will open up the full range of polymer and metal materials, allowing a more robust system design to withstand the rigors of flight, landing, and long term unattended operation on the surface of Mars.

Lueck, Dale E.↗

NASA NTRS2000

A Survey of Alternative Oxygen Production Technologies

Lueck, Dale E.↗

NASA NTRS2024

Fundamental Experimental Tests and Modeling of LOX/CH4 Engines at High Pressures

In recent years, the space travel industry has grown exponentially, resulting in the need for a low-cost, efficient rocket engine fuel. As such, there has been renewed interest in utilizing liquid natural gas (LNG) as it is less likely to soot than kerosene-based fuels and has widespread availability and low cost of use as compared to the traditional RP-X and even liquid methane (LCH4) fuels due to the reduced need for refinement. However, current literature does not fully cover varying blends of natural gas and the effects that impurities have on natural gas/methane fuels, with most studies being confined to low-pressure applications. Therefore, new experimental ignition delay time measurements at rocket engine relevant pressures are essential to ensure current chemical kinetic models capture the ignition behavior at these elevated conditions and to determine the optimal purity levels for a reliable, cost-efficient, aerospace-grade LCH4/LNG fuel. The current work explores various blends of natural gas/methane fuel with various impurities, including higher hydrocarbons as well as nitrogen-carriers. A shock tube study was carried out to study the ignition delay times and carbon monoxide time histories of these natural gas blends utilizing chemiluminescence and laser absorption spectroscopy at 20, 50 and 100 atm over temperatures ranging from 1400-1700K and at an equivalence ratio of 1. The experimental data was then compared to two different chemical kinetic mechanisms: the industry-standard GRI 3.0 and the in-house UCF 2022. The data is used to improve chemical kinetic mechanisms and modeling of LNG fuels for rocket engine applications.

Methane↗

DOE OSTI2021

Pore accessibility and trapping of methane in Marcellus shale

Accessibility of pore space in unconventional reservoirs is an important factor influencing both methane storage capacity and the kinetics of methane desorption. The determination of open (accessible) versus closed (inaccessible) porosity is therefore vital for the prediction of gas production potential. This study investigates accessibility of pores to methane in overmature middle Devonian Marcellus shale samples (cut parallel and perpendicular to bedding) using small and ultra-small neutron scattering (SANS and USANS) with contrast matching (CM), supplemented by other complementary techniques, such as mercury injection capillary pressure (MICP) and low pressure gas (N2 and CO2) adsorption. Our results demonstrate that for the samples studied, only about 6 % of pores with diameter 25-500 nm are accessible to methane. The accessibility fraction for pores larger than 500 nm is 35%. For nanopores smaller than 25 nm, pore accessibility could not be quantitatively determined due to increased methane density and condensation effects in confinement. Our observations indicate that methane penetrates the accessible small mesopores and micropores down to at least 1 nm in diameter, and the density of confined deuterated methane (CD4) is 0.68 g/cm3 for pores of diameter 25 nm and gradually increases with the decreased pore size. Moreover, elevated gas pressure causes formation of additional high-density methane nano-clusters. These clusters have a form of slightly anisotropic polydisperse discs oriented along bedding plane, about 1-12 nm in diameter and with average thickness of 3.6 nm. Utilizing samples cut parallel and perpendicular to the bedding, this study also briefly addresses anisotropy of pores. Based on the iso-size intensity ratio R, our SANS and USANS results demonstrate anisotropy in the out-of-bedding direction and suggest that the degree of anisotropy depends on the pore size. Specifically, for pore diameters ~2.5 to 250 nm, the extent of anisotropy is smaller than for pores ~500 nm to 6 µm in diameter. Finally, comparison of pore size distribution results calculated from SANS/USANS to those obtained using MICP shows good agreement at low pressures, but large difference at pressures above 1000 bar. Here, this discrepancy requires further testing; it is possible that the high mercury pressure used in MICP alters the mesopore and micropore structure of shales.

03 NATURAL GAS↗

NASA NTRS1998

Status of Liquid Oxygen/Liquid Methane Injector Study for a Mars Ascent Engine

Preliminary mission studies for human exploration of Mars have been performed at Marshall Space Flight Center (MSFC). These studies indicate that for non-toxic chemical rockets only a cryogenic propulsion system would provide high enough performance to be considered for a Mars ascent vehicle. Although the mission is possible with Earth-supplied propellants for this vehicle, utilization of in-situ propellants is highly attractive. This option would significantly reduce the overall mass of the return vehicle. Consequently, the cost of the mission would be greatly reduced because the number and size of the Earth launch vehicle(s) needed for the mission decrease. NASA/Johnson Space Center has initiated several concept studies (2) of in-situ propellant production plants. Liquid oxygen (LOX) is the primary candidate for an in-situ oxidizer. In-situ fuel candidates include methane (CH4), ethylene (C2H4), and methanol (CH3OH). MSFC initiated a technology development program for a cryogenic propulsion system for the Mars human exploration mission in 1998. One part of this technology program is the effort described here: an evaluation of propellant injection concepts for a LOX/liquid methane Mars Ascent Engine (MAE) with an emphasis on light-weight, high efficiency, reliability, and thermal compatibility. In addition to the main objective, hot-fire tests of the subject injectors will be used to test other key technologies including light-weight combustion chamber materials and advanced ignition concepts. This state-of-the-art technology will then be applied to the development of a cryogenic propulsion system that will meet the requirements of the planned Mars sample return (MSR) mission. The current baseline propulsion system for the MSR mission uses a storable propellant combination [monomethyl hydrazine/mixed oxides of nitrogen-25(MMH/MON-25)]. However, a mission option that incorporates in-situ propellant production and utilization for the ascent stage is being carefully considered as a subscale precursor to a future human mission to Mars.

Trinh, Huu Ogyic↗

DOE OSTI2025

Identification and evolution of active sites in isomorphously substituted Fe-ZSM-5 catalysts for methane dehydroaromatization (MDA)

Methane dehydroaromatization (MDA) enables the catalytic conversion of methane into aromatics, mainly benzene, along with hydrogen, in a single-step process under non-oxidative conditions. In this study, we prepared a series of isomorphously substituted Fe-ZSM-5 catalysts with exclusively isolated or low-oligomerized sites up to 3.2% Fe weight loading by adding ethylenediaminetetraacetic acid (EDTA) to the crystallization gel. These catalysts exhibit no induction/activation period and a significantly higher maximum product yield compared to Fe/ZSM-5 catalysts prepared by the incipient wetness impregnation method and containing extensively aggregated FeOx. This investigation focuses on the evolution of Fe sites during the post-synthetic treatments. Most importantly, we demonstrate the quantitative relation between Fe site isolation and catalytic activity, proving that isolated or low-oligomerized Fe species at the exchange sites formed during post-synthetic retreatment are the active sites for methane activation.

02 PETROLEUM↗

DOE OSTI2025

Diversity and Distribution of Hydrocarbon-Degrading Genes in the Cold Seeps from the Mediterranean and Caspian Seas

Marine cold seeps are unique ecological niches characterized by the emergence of hydrocarbons, including methane, which fosters diverse microbial communities. This study investigates the diversity and distribution of hydrocarbon-degrading genes and organisms in sediments from the Caspian and Mediterranean Seas, utilizing 16S rRNA and metagenomic sequencing to elucidate microbial community structure and functional potential. Our findings reveal distinct differences in hydrocarbon degrading gene profiles between the two seas, with pathways for aerobic and anaerobic hydrocarbon degradation co-existing in sediments from both basins. Aerobic pathways predominate in the surface sediments of the Mediterranean Sea, while anaerobic pathways are favored in the surface sediments of the anoxic Caspian Sea. Additionally, sediment depths significantly influence microbial diversity, with variations in gene abundance and community composition observed at different depths. Aerobic hydrocarbon-degrading genes decrease in diversity with depth in the Mediterranean Sea, whereas the diversity of aerobic hydrocarbon-degrading genes increases with depth in the Caspian Sea. These results enhance our understanding of microbial ecology in cold seep environments and have implications for bioremediation practices targeting hydrocarbon pollutants in marine ecosystems.

Microbiology↗

NASA NTRS1977

Alternate aircraft fuels prospects and operational implications

The paper discusses NASA studies of the potentials of coal-derived aviation fuels, specifically synthetic aviation kerosene, liquid methane, and liquid hydrogen. Topics include areas of fuel production, air terminal requirements for aircraft fueling (for liquid hydrogen only), and the performance characteristics of aircraft designed to utilize alternate fuels. Energy requirements associated with the production of each of the three selected fuels are determined, and fuel prices are estimated. Subsonic commercial air transports using liquid hydrogen fuel have been analyzed, and their performance and the performance of aircraft which use commercial aviation kerosene are compared. Environmental and safety issues are considered.

Witcofski, R. D.↗

DOE OSTI2024

Intensified Positive Arctic–Methane Feedback under IPCC Climate Scenarios in the 21st Century

The positive Arctic–methane (CH 4 ) feedback forms when more CH 4 is released from the Arctic tundra to warm the climate, further stimulating the Arctic to emit CH 4 . This study utilized the CLM-Microbe model to project CH 4 emissions across five distinct Arctic tundra ecosystems on the Alaska North Slope, considering three Shared Socioeconomic Pathway (SSP) scenarios using climate data from three climate models from 2016 to 2100. Employing a hyper-resolution of 5 m × 5 m within 40,000 m 2 domains accounted for the Arctic tundra’s high spatial heterogeneity; three sites were near $Utqia\dot{g}vik$ (US-Beo, US-Bes, and US-Brw), with one each in Atqasuk (US-Atq) and Ivotuk (US-Ivo). Simulated CH 4 emissions substantially increased by a factor of 5.3 to 7.5 under the SSP5–8.5 scenario compared to the SSP1–2.6 and SSP2–4.5 scenarios. The projected CH 4 emissions exhibited a stronger response to rising temperature under the SSP5–8.5 scenario than under the SSP1–2.6 and SSP2–4.5 scenarios, primarily due to strong temperature dependence and the enhanced precipitation-induced expansion of anoxic conditions that promoted methanogenesis. The CH 4 transport via ebullition and plant-mediated transport is projected to increase under all three SSP scenarios, and ebullition dominated CH 4 transport by 2100 across five sites. Projected CH 4 emissions varied in temperature sensitivity, with a Q 10 range of 2.7 to 60.9 under SSP1–2.6, 3.8 to 17.6 under SSP2–4.5, and 5.7 to 17.2 under SSP5–8.5. Compared with the other three sites, US-Atq and US-Ivo were estimated to have greater increases in CH 4 emissions due to warmer temperatures and higher precipitation. The fact that warmer sites and warmer climate scenarios had higher CH 4 emissions suggests an intensified positive Arctic–CH 4 feedback in the 21st century. Microbial physiology and substrate availability dominated the enhanced CH 4 production. The simulated intensified positive feedback underscores the urgent need for a more mechanistic understanding of CH 4 dynamics and the development of strategies to mitigate CH 4 across the Arctic.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1988

Quick actuating closure and handling system

A quick activating closure and handling system, which utilizes conical sections for locking, was developed to allow quick access to the combustor internal components of the 8 ft High Temperature Tunnel. These critical components include the existing methane spraybar, a transpiration cooled nozzle and the new liquid oxygen (LOX) injection system housed within the combustor. A substantial cost savings will be realized once the mechanism is installed since it will substantially reduce the access time and increase the time available for conducting wind tunnel tests. A need exists for more frequent inspections when the wind tunnel operates at the more severe conditions generated by using LOX in the combustor. A loads analysis and a structural (finite element) analysis were conducted to verify that the new closure system is compatible with the existing pressure shell. In addition, strain gages were placed on the pressure vessel to verify how the pressure shell reacts to transient pressure loads. A scale model of the new closure system was built to verify the operation of the conical sections in the locking mechanisms.

Allred, Johnny W.↗

NASA NTRS1994

Making Ceramic Components For Advanced Aircraft Engines

Lightweight, oxidation-resistant silicon nitride components containing intricate internal cooling and hydraulic passages and capable of withstanding high operating temperatures made by ceramic-platelet technology. Used to fabricate silicon nitride test articles of two types: components of methane-cooled regenerator for air turbo ramjet engine and components of bipropellant injector for rocket engine. Procedures for development of more complex and intricate components established. Technology has commercial utility in automotive, aircraft, and environmental industries for manufacture of high-temperature components for use in regeneration of fuels, treatment of emissions, high-temperature combustion devices, and application in which other high-temperature and/or lightweight components needed. Potential use in fabrication of combustors and high-temperature acoustic panels for suppression of noise in future high-speed aircraft.

Franklin, J. E.↗