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NASA NTRS2010

Sabatier Reactor System Integration with Microwave Plasma Methane Pyrolysis Post-Processor for Closed-Loop Hydrogen Recovery

The Carbon Dioxide Reduction Assembly (CRA) designed and developed for the International Space Station (ISS) represents the state-of-the-art in carbon dioxide reduction (CDRe) technology. The CRA produces water and methane by reducing carbon dioxide with hydrogen via the Sabatier reaction. The water is recycled to the Oxygen Generation Assembly (OGA) and the methane is vented overboard resulting in a net loss of hydrogen. The proximity to earth and the relative ease of logistics resupply from earth allow for a semi-closed system on ISS. However, long-term manned space flight beyond low earth orbit (LEO) dictates a more thoroughly closed-loop system involving significantly higher recovery of hydrogen, and subsequent recovery of oxygen, to minimize costs associated with logistics resupply beyond LEO. The open-loop ISS system for CDRe can be made closed-loop for follow-on missions by further processing methane to recover hydrogen. For this purpose, a process technology has been developed that employs a microwave-generated plasma to reduce methane to hydrogen and acetylene resulting in 75% theoretical recovery of hydrogen. In 2009, a 1-man equivalent Plasma Pyrolysis Assembly (PPA) was delivered to the National Aeronautics and Space Administration (NASA) for technical evaluation. The PPA has been integrated with a Sabatier Development Unit (SDU). The integrated process configuration incorporates a sorbent bed to eliminate residual carbon dioxide and water vapor in the Sabatier methane product stream before it enters the PPA. This paper provides detailed information on the stand-alone and integrated performance of both the PPA and SDU. Additionally, the integrated test stand design and anticipated future work are discussed.

Abney, Morgan B.↗

NASA NTRS2011

Reduced Pressure Cabin Testing of the Orion Atmosphere Revitalization Technology

An amine-based carbon dioxide (CO2) and water vapor sorbent in pressure-swing regenerable beds has been developed by Hamilton Sundstrand and baselined for the Atmosphere Revitalization System for moderate duration missions of the Orion Multipurpose Crew Vehicle. In previous years at this conference, reports were presented on extensive Johnson Space Center testing of this technology in a sea-level pressure environment with simulated and actual human metabolic loads in both open and closed-loop configurations. In 2011, the technology was tested in an open cabin-loop configuration at ambient and two sub-ambient pressures to compare the performance of the system to the results of previous tests at ambient pressure. The testing used a human metabolic simulator with a different type of water vapor generation than previously used, which added some unique challenges in the data analysis. This paper summarizes the results of: baseline and some matrix testing at all three cabin pressures, increased vacuum regeneration line pressure with a high metabolic load, a set of tests studying CO2 and water vapor co-adsorption effects relative to model-predicted performance, and validation tests of flight program computer model predictions with specific operating conditions.

Button, Amy↗

NASA NTRS2011

The Orion Atmosphere Revitalization Technology in Manned Ambient Pressure Space Suit Testing

An amine-based carbon dioxide (CO2) and water vapor sorbent in pressure-swing regenerable beds has been developed by Hamilton Sundstrand and baselined for the Atmosphere Revitalization System (ARS) for moderate duration missions of the Orion Multipurpose Crew Vehicle. The Orion ARS is designed to support not only open-cabin operations, tests of which have been reported in previous years at this conference, but also closed space suit-loop operations. A previous low-pressure suit loop test was performed with a human metabolic simulator, and humans wearing emergency masks were tested in a closed-loop configuration before that. In late 2011, simple tests were performed in a suit-loop configuration with human test subjects in prototype space suits with prototype umbilicals at ambient and two slightly above-ambient pressures. Trace contaminant filters and a prototype blower were also incorporated into the test rig. This paper discusses the performance of the ARS technology in that 2011 test configuration.

Button, Amy↗

NASA NTRS2013

Reduced Pressure Cabin Testing of the Orion Atmosphere Revitalization Technology

Button, Amy↗

NASA NTRS2013

Reduced Pressure Cabin Testing of the Orion Atmosphere Revitalization Technology

An amine-based carbon dioxide (CO2) and water vapor sorbent in pressure-swing regenerable beds has been developed by United Technologies Corp. Aerospace Systems (UTAS, formerly Hamilton Sundstrand) and baselined for the Atmosphere Revitalization System for moderate duration missions of the Orion Multipurpose Crew Vehicle (MPCV). In previous years at this conference, reports were presented on extensive Johnson Space Center testing of this technology in a sea-level pressure environment with simulated and actual human metabolic loads in both open and closed-loop configurations. In 2011, the technology was tested in an open cabin-loop configuration at ambient and two sub-ambient pressures to compare the performance of the system to the results of previous tests at ambient pressure. The testing used a human metabolic simulator with a different type of water vapor generation than previously used, which added some unique challenges in the data analysis. This paper summarizes the results of: baseline and some matrix testing at all three cabin pressures, increased vacuum regeneration line pressure testing with a high metabolic load, a set of tests studying CO2 and water vapor co-adsorption effects relative to model-predicted performance, and validation tests of flight project computer model predictions with specific operating conditions.

Button, Amy B.↗

NASA NTRS2016

NASA Advanced Explorations Systems: Advancements in Life Support Systems

The NASA Advanced Exploration Systems (AES) Life Support Systems (LSS) project strives to develop reliable, energy-efficient, and low-mass spacecraft systems to provide environmental control and life support systems (ECLSS) critical to enabling long duration human missions beyond low Earth orbit (LEO). Highly reliable, closed-loop life support systems are among the capabilities required for the longer duration human space exploration missions assessed by NASA's Habitability Architecture Team (HAT). The LSS project is focused on four areas: architecture and systems engineering for life support systems, environmental monitoring, air revitalization, and wastewater processing and water management. Starting with the international space station (ISS) LSS systems as a point of departure (where applicable), the mission of the LSS project is three-fold: 1. Address discrete LSS technology gaps 2. Improve the reliability of LSS systems 3. Advance LSS systems towards integrated testing on the ISS. This paper summarized the work being done in the four areas listed above to meet these objectives. Details will be given on the following focus areas: Systems Engineering and Architecture- With so many complex systems comprising life support in space, it is important to understand the overall system requirements to define life support system architectures for different space mission classes, ensure that all the components integrate well together and verify that testing is as representative of destination environments as possible. Environmental Monitoring- In an enclosed spacecraft that is constantly operating complex machinery for its own basic functionality as well as science experiments and technology demonstrations, it's possible for the environment to become compromised. While current environmental monitors aboard the ISS will alert crew members and mission control if there is an emergency, long-duration environmental monitoring cannot be done in-orbit as current methodologies rely largely on sending environmental samples back to Earth. The LSS project is developing onboard analysis capabilities that will replace the need to return air and water samples from space for ground analysis. Air Revitalization- The air revitalization task is comprised of work in carbon dioxide removal, oxygen generation and recovery and trace contamination and particulate control. The CO2 Removal and associated air drying development efforts under the LSS project are focused both on improving the current SOA technology on the ISS and assessing and examining the viability of other sorbents and technologies available in academia and industry. The Oxygen Generation and Recovery technology development area encompasses several sub-tasks in an effort to supply O2 to the crew at the required conditions, to recover O2 from metabolic CO2, and to recycle recovered O2 back to the cabin environment. Current state-of-the-art oxygen generation systems aboard space station are capable of generating or recovering approximately 40% of required oxygen; for exploration missions this percentage needs to be greatly increased. A spacecraft cabin trace contaminant and particulate control system serves to keep the environment below the spacecraft maximum allowable concentration (SMAC) for chemicals and particulates. Both passive (filters) and active (scrubbers) methods contribute to the overall TC & PC design. Work in the area of trace contamination and particulate control under the LSS project is focused on making improvements to the SOA TC & PC systems on ISS to improve performance and reduce consumables. Wastewater Processing and Water Management- A major goal of the LSS project is the development of water recovery systems to support long duration human exploration beyond LEO. Current space station wastewater processing and water management systems distill urine and wastewater to recover water from urine and humidity condensate in the spacecraft at a approximately 74% recovery rate. For longer, farther missions into deep space, that recovery rate must be greatly increased so that astronauts can journey for months without resupply cargo ships from Earth.

Shull, Sarah A.↗

DOE OSTI2026

Innovations Driven by Advanced Characterization to Strategize Critical Mineral Production and Beneficial Reuse from Fossil Energy Waste

Critical minerals (CM), such as rare earth elements (REE), cobalt, nickel, and lithium, have important uses in modern electronics and advanced manufacturing, yet are vulnerable to potential supply chain disruptions. Relatively abundant and readily available fossil energy (FE) wastes, such as coal combustion ash, acid mine drainage (AMD) and treatment solids (AMD solids), and Oil and Gas (O&G) drilling wastes (drill cuttings and produced waters) are under consideration as CM feedstocks. The National Energy Technology Laboratory (NETL) has studied CM resources for various FE wastes as part of the U.S. Department of Energy’s mission of bolstering the domestic CM supply, and makes the data available to the public on EDX at sites such as the NEWTS group. Advanced characterization utilizing synchrotron x-ray techniques coupled with laboratory extractions has been performed to identify CM hosting phases in these FE wastes to inform CM recoverability mechanisms. Novel methods to selectively recover CMs while co-producing other valuable byproducts have been developed. Successful examples discussed here include: (1) The identification of REE/Co/Ni/Sc binding and hosting phases in select FE waste (coal combustion ash and AMD solids), resulting in the development of a patented CM step-extraction process, (2) coupled production of functional sorbents from these extraction wastes and for CM recovery. A pilot-scale testing to evaluate the patent’s technical feasibility for extracting REE from coal ash on a barrel scale has been successfully performed. Additionally, (3) evaluation and measurements of brine geochemistry from U.S. O&G produced waters has informed a high Li recovery potential from Marcellus Shale produced water. NETL researchers have been developing tailored pre-treatment processes, an innovative and highly durable lithium sorbent, and geochemical model guided precipitation to accelerate Li production from the Marcellus Shale produced waters. These innovations driven by characterization are integral for maximizing and advancing the potential for CM recovery while offsetting the cost and environmental footprint for FE waste management.

critical mineral processing↗

NASA NTRS1974

Environmental carbon dioxide control

A study of environmental carbon dioxide control for NASA EVA missions found solid potassium carbonate to be an effective regenerable absorbent in maintaining low carbon dioxide levels. The supported sorbent was capable of repeated regeneration below 150 C without appreciable degradation. Optimum structures in the form of thin pliable sheets of carbonate, inert support and binder were developed. Interpretation of a new solid-gas pore closing model helped predict the optimum sorbent and analysis of individual sorbent sheet performance in a thin rectangular channel sorber can predict packed bed performance.

Onischak, M.↗

NASA NTRS2010

Sorbent, Sublimation, and Icing Modeling Methods: Experimental Validation and Application to an Integrated MTSA Subassembly Thermal Model

This paper details the validation of modeling methods for the three core components of a Metabolic heat regenerated Temperature Swing Adsorption (MTSA) subassembly, developed for use in a Portable Life Support System (PLSS). The first core component in the subassembly is a sorbent bed, used to capture and reject metabolically produced carbon dioxide (CO2). The sorbent bed performance can be augmented with a temperature swing driven by a liquid CO2 (LCO2) sublimation heat exchanger (SHX) for cooling the sorbent bed, and a condensing, icing heat exchanger (CIHX) for warming the sorbent bed. As part of the overall MTSA effort, scaled design validation test articles for each of these three components have been independently tested in laboratory conditions. Previously described modeling methodologies developed for implementation in Thermal Desktop and SINDA/FLUINT are reviewed and updated, their application in test article models outlined, and the results of those model correlations relayed. Assessment of the applicability of each modeling methodology to the challenge of simulating the response of the test articles and their extensibility to a full scale integrated subassembly model is given. The independent verified and validated modeling methods are applied to the development of a MTSA subassembly prototype model and predictions of the subassembly performance are given. These models and modeling methodologies capture simulation of several challenging and novel physical phenomena in the Thermal Desktop and SINDA/FLUINT software suite. Novel methodologies include CO2 adsorption front tracking and associated thermal response in the sorbent bed, heat transfer associated with sublimation of entrained solid CO2 in the SHX, and water mass transfer in the form of ice as low as 210 K in the CIHX.

Bower, Chad↗

DOE OSTI2026

Understanding and mitigating degradation in amine-based sorbents for CO 2 direct air capture

The success of direct air capture (DAC) of CO 2 depends on sorbents that combine high capacity, low energy requirements, and long-term durability. Amine-based sorbents-including solid-supported aminopolymers, grafted amines, and amine-functionalized resins-remain the leading candidates, but their limited lifetimes drive up costs and constrain deployment. In this review, we outline the current understanding of amine-based sorbent degradation with an emphasis on clearly identifying what is known about structure-property-performance relationships, as well as important knowledge gaps. More specifically, we discuss how polymer chemistry, sorbent design variables, and environmental and process conditions contribute to performance loss. In parallel, we outline how advances in spectroscopy, modeling, and accelerated testing are beginning to illuminate chemical and physical degradation mechanisms. Looking forward, we identify future research directions that will be critical for gaining a deeper understanding of degradation, as well as opportunities for developing innovative mitigation strategies for improving the lifetime of amine-based sorbents.

organic↗

NASA NTRS2015

Continued Advancement of Supported Liquid Membranes for Carbon Dioxide Control in Extravehicular Activity Applications

The Development of a new, robust, portable life support system (PLSS) is currently a high NASA priority in order to support longer and safer extravehicular activity (EVA) missions that will be necessary as space travel extends to near-Earth asteroids and eventually Mars. One of the critical PLSS functions is maintaining the carbon dioxide (CO2) concentration in the suit at acceptable levels. The Metal Oxide (MetOx) canister has a finite CO2 adsorption capacity and therefore in order to extend mission times, the unit would have to be larger and heavier, which is undesirable; therefore new CO2 control technologies must be developed. While recent work has centered on the use of alternating sorbent beds that can be regenerated during the EVA, this strategy increases the system complexity and power consumption. A simpler approach is to use a membrane that vents CO2 to space but retains oxygen(O2). A membrane has many advantages over current technology: it is a continuous system with no theoretical capacity limit, it requires no consumables, and it requires no hardware for switching beds between absorption and regeneration. Conventional gas separation membranes do not have adequate selectivity for use in the PLSS, but the required performance could be obtained with a supported liquid membrane (SLM), which consists of a microporous film filled with a liquid that selectively reacts with CO2 over oxygen (O2). In a recently completed Phase II Small Business Innovative Research project, Reaction Systems developed a new reactive liquid that has effectively zero vapor pressure, making it an ideal candidate for use in an SLM. Results obtained with the SLM in a flat sheet configuration with representative pressures of CO2, O2, and water (H2O) have shown that the CO2 permeation rate and CO2/O2 selectivity requirements have been met. In addition, the SLM vents moisture to space very effectively. The SLM has also been prepared and tested in a hollow fiber form, which will be necessary to meet size requirements in the PLSS. In initial tests, the required CO2 permeance values have been obtained, while the current CO2/O2 selectivity values are somewhat lower than needed. However, the performance of the SLM is a strong function of the method used to impregnate the sorbent in the hollow fiber walls and rapid progress is being made in that area.

Wickham, David T.↗

NASA NTRS2012

Developments in Atmosphere Revitalization Modeling and Simulation

"NASA's Advanced Exploration Systems (AES) program is pioneering new approaches for rapidly developing prototype systems, demonstrating key capabilities, and validating operational concepts for future human missions beyond Earth orbit" (NASA 2012). These forays beyond the confines of earth's gravity will place unprecedented demands on launch systems. They must not only blast out of earth's gravity well as during the Apollo moon missions, but also launch the supplies needed to sustain a crew over longer periods for exploration missions beyond earth's moon. Thus all spacecraft systems, including those for the separation of metabolic carbon dioxide and water from a crewed vehicle, must be minimized with respect to mass, power, and volume. Emphasis is also placed on system robustness both to minimize replacement parts and ensure crew safety when a quick return to earth is not possible. Current efforts are focused on improving the current state-of-the-art systems utilizing fixed beds of sorbent pellets by evaluating structured sorbents, seeking more robust pelletized sorbents, and examining alternate bed configurations to improve system efficiency and reliability. These development efforts combine testing of sub-scale systems and multi-physics computer simulations to evaluate candidate approaches, select the best performing options, and optimize the configuration of the selected approach, which is then implemented in a full-scale integrated atmosphere revitalization test. This paper describes the development of atmosphere revitalization models and simulations. A companion paper discusses the hardware design and sorbent screening and characterization effort in support of the Atmosphere Revitalization Recovery and Environmental Monitoring (ARREM) project within the AES program.

Knox, James C.↗

DOE OSTI2025

CO2-Utilization Facilitated by Solid Reaction Mediums—A Review

Abstract This short review examines solid reaction mediums—specifically oxygen, CO 2 , and carbon carriers—within the framework of Chemical Looping (CL) to illuminate various CO 2 utilization pathways. The thermodynamic consideration for carrier selection is first discussed. This is followed by a summary of the key carrier types investigated to date, with an emphasis on elucidating the roles of compositional, structural, and surface properties of the various carriers toward their reactive performances. Besides assessing the performances of various oxygen carriers, their long-term performance, potential deactivation mechanism in the presence of CO 2, and strategies for their reactivation are also discussed in the context of chemical looping dry reforming of methane (CLDRM). While relatively underexplored, the current status of development, advantages, and potential limitations of CO 2 carriers in sorbent looping dry reforming of methane (SLDRM) and carbon carriers in chemical looping methane cracking (CLMC) are also reviewed and discussed. Emerging topics such as combined carriers are also covered along with a perspective for future research directions. Overall, this review aims to offer insights into the sustainable use of CO 2 through chemical looping, emphasizing the potential of solid reaction mediums across different carriers and the challenges associated with these solid reaction mediums.

Iftikhar, Sherafghan↗

DOE OSTI2024

Polyamide-Based Ion Exchange Membranes: Cation-Selective Transport through Water Purification Membranes

Ion-selective membranes are necessary components of many electrochemical systems including fuel cells, electrolyzers, redox flow batteries, and electrodialyzers. Perfluorinated sulfonated membranes (PFSMs) dominate these applications due to their excellent combination of fast ion transport, stability, and processability. However, perfluorinated cation exchange membranes (CEMs) are expensive, and their production process involves chemistry that generates toxic perfluorinated chemicals. The development of affordable, nonfluorinated membranes with a competitive combination of high ion selectivity, transport, and stability could help enable the widespread use of the technologies listed above while hastening the development of emerging electrochemical systems, including aqueous alkaline CO 2 sorbent regeneration. To this end, we pursue the use of thin-film composite polyamide (PA-TFCs) membranes–those that typically find application in reverse osmosis and nanofiltration desalination–as cation-selective exchange membranes. Given their negative surface charge under neutral-to-alkaline conditions, PA-TFCs can serve as effective CEMs in these pH regimes. We prepared a series of PA-TFCs from traditional monomers (trimesoyl chloride and piperazine) and compared their thicknesses, charge densities, water transport properties, ion transport properties, and long-term stability in a high pH environment to traditional CEMs (Nafion and FKE) and commercial nanofiltration and reverse osmosis membranes. We find that some of the best-performing PA-TFC membranes have similar resistances and Na + transference numbers compared to Nafion 117 in Na 2 SO 4 and NaHCO 3 -containing solutions. This proof-of-principle study suggests that further optimization of PA-TFCs could enable cost-effective ion exchange membrane alternatives to PFSMs.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Energy-Efficient Direct Air Capture System for High Purity CO 2 Separation

The primary objective of this project is to demonstrate the University of Cincinnati’s direct air capture (DAC) sorbent technology in a monolithic structure installed in a passive air contactor (PAC). The modified amine-based sorbent technology provides reduced heat of desorption and resistance to thermal and oxidative degradations for robust and long-term performances and cost effective sorbent management. During the project period, additional amine modifications were developed and a U.S./PCT patent application was filed.

42 ENGINEERING↗

NASA NTRS2012

Development of Carbon Dioxide Removal Systems for Advanced Exploration Systems

"NASA's Advanced Exploration Systems (AES) program is pioneering new approaches for rapidly developing prototype systems, demonstrating key capabilities, and validating operational concepts for future human missions beyond Earth orbit" (NASA 2012). These forays beyond the confines of earth's gravity will place unprecedented demands on launch systems. They must not only blast out of earth's gravity well as during the Apollo moon missions, but also launch the supplies needed to sustain a crew over longer periods for exploration missions beyond earth's moon. Thus all spacecraft systems, including those for the separation of metabolic carbon dioxide and water from a crewed vehicle, must be minimized with respect to mass, power, and volume. Emphasis is also placed on system robustness both to minimize replacement parts and ensure crew safety when a quick return to earth is not possible. Current efforts are focused on improving the current state-of-the-art systems utilizing fixed beds of sorbent pellets by seeking more robust pelletized sorbents, evaluating structured sorbents, and examining alternate bed configurations to improve system efficiency and reliability. These development efforts combine testing of sub-scale systems and multi-physics computer simulations to evaluate candidate approaches, select the best performing options, and optimize the configuration of the selected approach, which is then implemented in a full-scale integrated atmosphere revitalization test. This paper describes the carbon dioxide (CO2) removal hardware design and sorbent screening and characterization effort in support of the Atmosphere Resource Recovery and Environmental Monitoring (ARREM) project within the AES program. A companion paper discusses development of atmosphere revitalization models and simulations for this project.

Knox, James C.↗

DOE OSTI2022

Developing Inorganic Resins for Radium and Actinium Generators and Purifications

The inorganic, normal-phase sorbents alumina, titania, and zirconia were evaluated and screened for the separation of Ba, La, 228 Ra, 228 Ac, and 212 Pb in a dilute acid matrix. The results show that the sorbents are capable of fractionating the ions between pH 1–8. Acetate and total metal ion concentrations were experimentally evaluated as factors that could affect retention using La and Ba surrogates. Pseudo-second order rate constants were derived and the uptake of La was determined to be endothermic. A stationary zirconia column was used to isolate Ba from La and Ra from Ac/Pb; elution profiles of each separation are presented. The utility and implications of these sorbents are discussed with respects to large-scale production of 225 Ac from radium targets. This work was published in 2020 and in 2022.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

NASA NTRS2000

Numerical Simulation of a Chemically Reacting Sorbent Bed for LSS Applications

A detailed numerical model of a chemisorption bed has been developed. The model is based on the constant pressure mass transport equation for gaseous flow through a packed bed, and the equation for diffusion and reaction within a spherical particle. Because there is a wealth of data from the NASA and the Navy bodies of literature, the LiOH-H2O-CO2 system is chosen for application of the model and interpretation of results. Prior models of this system from the life support literature are limited. The current model incorporates many of the features of elaborate models developed for investigation of industrial systems or energy applications (e.g., coal, desulphurization): it distinguishes bulk convection and bed dispersion; mass transport to the particle surface, transport within the particle, and reaction. It uses the nonsteady (not pseudo-steady state) form of the equations. The chemistry is modeled as a multi-step, reversible reaction with evolving solid structure. The resulting system of equations is large. The ODEPACK family of solvers is used to integrate the system. Reaction coefficients are determined by experiment. Typical results of the model are illustrated with mission input parameters. Using the model, an explanation is offered for 1) the varied performance results found after pre-breathing (or after simulated pre-breathe conditions), 2) interrupted use and 3) low temperature use. In addition, options for a reusable canister are explored. The computational resource implications of adding energy equations are discussed briefly, as are applicability to other relevant space and undersea systems.

Luna, Bernadette↗