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DOE OSTI2024

CFD Model Development of a Small-Scale Fixed-Bed Reactor for Direct Air Capture of CO2

Direct air capture (DAC) is a promising approach to significantly reduce the CO2 concentration in the ambient air. This approach requires the extraction of CO2 from air with ultra dilute CO2 concentration which makes this approach more expensive than point source CO2 capture. Several efforts are being made in academics and industry to develop cost-efficient sorbents and solvents suitable for DAC. One of them is polymer with intrinsic microporosity (PIM) which is often used for CO2 capture because of its higher porosity and rigidity. A novel, cost-efficient aminated PIM sorbent, PF-15-TAEA, was developed at the National Energy Technology Laboratory for DAC applications. The current work is focused on the computational investigation of the CO2 capture by this novel sorbent from a gas mixture with ultra dilute concentration of CO2 in dry and humid conditions in a laboratory-scale fixed-bed reactor.

Aziz, Hossain↗

DOE OSTI2021

Iodine Sorption on AgZ-PAN

The Department of Energy (DOE) Nuclear Fuel Cycle and Supply Chain Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has performed research and development on iodine control and iodine waste forms for the past several years. This research and development has included iodine adsorption tests using a laboratory-scale test system containing multiple-segmented fixed beds of iodine adsorbents. Iodine capture performance has been tested using (a) non-radioactive synthetic gas mixtures blended from air, nitrogen, NO, NO 2 , water, to simulate dissolver off-gas (DOG) and vessel off-gas (VOG) streams from used nuclear fuel aqueous reprocessing, (b) inorganic and organic iodine species, and (c) different sorbents. An initial test of silver-functionalized mordenite in polyacrylonitrile matrix (AgZ-PAN) was conducted to assess if this sorbent, initially designed for selective sorption of Xe that evolves into used fuel reprocessing off-gas streams, could also be a candidate for iodine sorption. This test was conducted using the same deep-bed test system and methodologies used in many prior iodine sorption tests using other sorbents. Diatomic iodine (I2) was used as the target iodide in a gas stream containing air, NO, NO 2 , and moisture designed to simulate an aqueous reprocessing dissolver off-gas (DOG) stream.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

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↗

DOE OSTI2020

Evaluation of Engineered Form MOFs CaSDB and HKUST-1

Idaho National Laboratory (INL) and Pacific Northwest National Laboratory (PNNL) have studied different sorbents for the purpose of separating krypton (Kr) and xenon (Xe). PNNL has researched various metal-organic frameworks (MOFs) that have characteristics theoretically suitable for the separation. Based on computational analysis, PNNL chose Calcium–4,4’–sulfonyl dibenzoate (CaSDB) and Hong Kong University of Science and Technology MOF1 (HKUST–1). The raw MOFs are supplied in a powder form and must be incorporated into a robust engineered form to be viable for gas separation. In 2016, PNNL produced an engineered form of CaSDB by compressing and grinding the raw MOF material. This form was sent to INL for adsorption testing. Gentle mechanical agitation of the compressed form produced a large amount of powder, resulting in the conclusion that the form was not viable for the application. In 2019, INL successfully produced two engineered forms, CaSDB–EF1 and HKUST–EF2, by incorporating the active MOF powders into a polyacrylonitrile (PAN) binder. PNNL also produced two engineered forms, CaSDB–10pmma and HKUST–10pmma, by using polymethyl methacrylate (PMMA) as a binder. Surface area analysis indicated that the forms could be viable for separations in which the CaSDB–EF1 retained 84% of the raw CaSDB surface area and CaSDB–10pmma retained 48%. HKUST–EF2 retained all the raw HKUST–1 surface area, whereas HKUST–10pmma retained only 28%. Mechanical stability testing demonstrated that the PMMA forms formed a fine powder whereas, the PAN forms did not. In general, adsorption testing showed that CaSDB–10pmma had a lower Xe breakthrough capacity than CaSDB–EF1, but a higher saturation capacity at both room temperature and at 253 K. The CaSDB MOF was intended to be used as a room temperature sorbent to capture Xe. However, both CaSDB engineered forms displayed relatively short initial break through times. Reduced temperature increased the Xe capacity of both engineered forms. HKUST–1 was expected to be effective only at sub-zero temperatures. At 195 K, HKUST–10pmma had an initial Xe breakthrough capacity of 119 mmol/ kg, compared to HKUST–EF2 at 339 mmol/ kg. The saturation capacities were 275 and 383 mmol/ kg, respectively. HKUST–10ppm also had a lower Kr capacity of 1.7 mmol/kg, whereas the HKUST–EF had a Kr capacity of 3 mmol/ kg. Test results indicate that the PAN engineered forms are a more suitable choice for the complete separation of Xe and Kr, due to the increase in initial breakthrough capacity. CaSDB allows rapid breakthrough of Kr and Xe regardless of the type of engineered form. At 253 K, it is more viable, but is still not the most effective sorbent. HKUST–EF2 demonstrated viability for Xe capture at 195 K, which may merit further study, however it may be cost prohibitive.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Evaluating Polymer Properties with Different Additives for Carbon Capture and Other Applications

Anthropogenic climate change is one of this generation’s most pressing concerns, with the potential to completely alter the delicate balance we’ve struck with nature. Already, global temperatures have risen 1.29°C, leading to disrupted weather systems, extinctions, increased risks of wildfires, and sea level rise, to name a few effects. Carbon dioxide emission from the combustion of fossil fuels and other industrial activity is a large driver of this phenomenon, as it absorbs heat before it can be radiated away from Earth, trapping it. Carbon dioxide has reached unprecedented levels in our atmosphere, showing a 50% increase from preindustrial averages to a whopping 430 ppm. Thus, reducing the amount of carbon dioxide via carbon capture technology is an important endeavor that serves to benefit everyone. The Microencapsulated CO 2 Sorbent (MECS) team at Lawrence Livermore National Laboratory (LLNL) has turned to microencapsulation to approach this endeavor. Microcapsules provide an attractive approach to carbon capture, combining large surface areas for more efficient mass transfer, regenerative abilities, reduced solvent loss, and improved handling. Additionally, while existing carbon capture technology relies on industrial plants, capsules could present a modular approach to carbon capture, reducing the need for extensive physical infrastructure. The MECS team’s design consists of a polymer membrane that contains a liquid carbon sequestering sorbent, aqueous sodium carbonate. The carbon capturing reaction occurs in three distinct steps, the first of which is the dissolution of carbon dioxide into the sorbent solution and its conversion into carbonic acid (H 2 CO 3 ), shown in equations 1 and 2 respectively. Because this step hinges upon the ability of carbon dioxide to reach the solution inside the capsule, it is necessary that the microcapsule shell is permeable to carbon dioxide gas. The MECS team produces these microcapsules using the in-air droplet encapsulation apparatus (IDEA) shown in figure 1, which can produce uniform micron-scale droplets at speeds much faster than traditional single-dispersal microfluidic-based techniques. The IDEA Is 100 times faster than these current techniques and can reach up to 1000 times their speed when incorporating a multi-nozzle design. Additionally, because droplets are produced in-air via vibration, IDEA can decrease post-processing times and material waste by 99% and can fabricate microgels that are 10 to 100 times more viscous than can be produced via traditional microfluidics. While this design represents a breakthrough in the throughput, efficiency, and tunability of microcapsule production, it imposes a major constraint on the microcapsule curing process. Because microcapsule shells are crosslinked with UV light while falling 30 cm through the air, this gives them a reaction window of approximately 0.2 seconds. Thus, the system and shell formulations must be optimized such that the shells can be fully crosslinked within this very narrow window, prompting investigations into curing behavior.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Abatement of radioiodine in aqueous reprocessing off-gas

The reprocessing used nuclear fuel (UNF) releases volatile fission and activation products, including 129 I, into the off-gas of a processing plant. Mitigation of the release of vapor phase radionuclides is necessary for meeting regulatory requirements in the United States and other countries. In an aqueous reprocessing plant, volatile radioiodine could be present in several forms, depending on the chemistry of the process used. Inorganic iodine will be the predominate species in any shearing or voloxidation pretreatment off-gas and dissolver off-gas (DOG). Organic iodides such as CH 3 I, C 4 H 9 I, and C 12 H 25 I have been proposed to be generated during solvent extraction; thus, these species must be captured from the vessel off-gas (VOG). The abatement of inorganic and organic iodide species to meet United States regulatory requirements has been demonstrated in laboratory experiments using Ag-based solid sorbents. The data presented in this paper includes the effect of gas composition (e.g., the presence of water vapor and NO x ), iodine speciation (I 2 , CH 3 I, C 4 H 9 I, C 12 H 25 I), and sorbent bed parameters (e.g., temperature, sorbent age) on complete iodine capture on Ag-mordenite in an aqueous reprocessing plant.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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 NTRS1980

Factors affecting cleanup of exhaust gases from a pressurized, fluidized-bed coal combustor

The cleanup of effluent gases from the fluidized-bed combustion of coal is examined. Testing conditions include the type and feed rate of the coal and the sulfur sorbent, the coal-sorbent ratio, the coal-combustion air ratio, the depth of the reactor fluidizing bed, and the technique used to physically remove fly ash from the reactor effluent gases. Tests reveal that the particulate loading matter in the effluent gases is a function not only of the reactor-bed surface gas velocity, but also of the type of coal being burnt and the time the bed is operating. At least 95 percent of the fly ash particules in the effluent gas are removed by using a gas-solids separator under controlled operating conditions. Gaseous pollutants in the effluent (nitrogen and sulfur oxides) are held within the proposed Federal limits by controlling the reactor operating conditions and the type and quantity of sorbent material.

Rollbuhler, R. J.↗

NASA NTRS1995

Molecular Sieve Bench Testing and Computer Modeling

The design of an efficient four-bed molecular sieve (4BMS) CO2 removal system for the International Space Station depends on many mission parameters, such as duration, crew size, cost of power, volume, fluid interface properties, etc. A need for space vehicle CO2 removal system models capable of accurately performing extrapolated hardware predictions is inevitable due to the change of the parameters which influences the CO2 removal system capacity. The purpose is to investigate the mathematical techniques required for a model capable of accurate extrapolated performance predictions and to obtain test data required to estimate mass transfer coefficients and verify the computer model. Models have been developed to demonstrate that the finite difference technique can be successfully applied to sorbents and conditions used in spacecraft CO2 removal systems. The nonisothermal, axially dispersed, plug flow model with linear driving force for 5X sorbent and pore diffusion for silica gel are then applied to test data. A more complex model, a non-darcian model (two dimensional), has also been developed for simulation of the test data. This model takes into account the channeling effect on column breakthrough. Four FORTRAN computer programs are presented: a two-dimensional model of flow adsorption/desorption in a packed bed; a one-dimensional model of flow adsorption/desorption in a packed bed; a model of thermal vacuum desorption; and a model of a tri-sectional packed bed with two different sorbent materials. The programs are capable of simulating up to four gas constituents for each process, which can be increased with a few minor changes.

Mohamadinejad, Habib↗

NASA NTRS1996

Microwave Regenerable Air Purification Device

The feasibility of using microwave power to thermally regenerate sorbents loaded with water vapor, CO2, and organic contaminants has been rigorously demonstrated. Sorbents challenged with air containing 0.5% CO2, 300 ppm acetone, 50 ppm trichloroethylene, and saturated with water vapor have been regenerated, singly and in combination. Microwave transmission, reflection, and phase shift has also been determined for a variety of sorbents over the frequency range between 1.3-2.7 GHz. This innovative technology offers the potential for significant energy savings in comparison to current resistive heating methods because energy is absorbed directly by the material to be heated. Conductive, convective and radiative losses are minimized. Extremely rapid heating is also possible, i.e., 1400 C in less than 60 seconds. Microwave powered thermal desorption is directly applicable to the needs of Advance Life Support in general, and of EVA in particular. Additionally, the applicability of two specific commercial applications arising from this technology have been demonstrated: the recovery for re-use of acetone (and similar solvents) from industrial waste streams using a carbon based molecular sieve; and the separation and destruction of trichloroethylene using ZSM-5 synthetic zeolite catalyst, a predominant halocarbon environmental contaminant. Based upon these results, Phase II development is strongly recommended.

Atwater, James E.↗

NASA NTRS2006

Testing of an Amine-Based Pressure-Swing System for Carbon Dioxide and Humidity Control

Hamilton Sundstrand has developed a stable and efficient amine-based carbon dioxide (CO2) and water vapor (H2O) sorbent, SA9T, that is well-suited for use in a spacecraft environment. The sorbent is efficiently packaged in pressure-swing regenerable beds that are thermally linked to improve removal efficiency and minimize vehicle thermal loads, and the flows are all controlled with a single spool valve. The SA9T sorbent technology has already been baselined for the new Orion spacecraft. However, more data was needed on the operational characteristics of the package in a simulated spacecraft environment. This amine-based technology, referred to as the CO2 And Moisture Removal Amine Swing-bed (CAMRAS) by the Exploration Life Support Air Team at Johnson Space Center (JSC), was tested at JSC during the last third of 2006. Two series of tests on the CAMRAS were performed at simulated metabolic loads of four and/or six crewmen in a closed chamber. Tests were run at a variety of cabin temperatures and with a range of operating conditions varying cycle time, available vacuum pressure, blower speed, and crew activity levels. Results of this testing are presented and potential flight operational strategies discussed.

Lin, Amy B.↗

NASA NTRS2009

PLSS Scale Demonstration of MTSA Temperature Swing Adsorption Bed Concept for CO2 Removal/Rejection

Metabolic heat regenerated temperature swing adsorption (MTSA) incorporated into a portable life support system (PLSS) is being explored as a viable means of removing and rejecting carbon dioxide (CO2) from an astronaut s ventilation loop. Sorbent pellets used in previous work are inherently difficult to quickly heat and cool. Further, their use in packed beds create large undesirable pressure drop. Thus work has been done to assess the application and performance of aluminum foam wash coated with a layer of sorbent. A to-scale sorbent bed, as envisioned studying use by a Martian PLSS, was designed, built, and tested. Performance of the assembly in regards to CO2 adsorption and pressure drop were assessed and the results are presented.

Iacomini, Christine S.↗

NASA NTRS2010

Carbon Dioxide Control System for a Mars Space Suit Life Support System

Carbon dioxide (CO2) control during Extravehicular Activities (EVAs) on Mars will be challenging. Lithium hydroxide (LiOH) canisters have impractical logistics penalties, and regenerable metal oxide (MetOx) canisters weigh too much. Cycling bed systems and permeable membranes that are regenerable in space vacuum cannot vent on Mars due to the high partial pressure of CO2 in the atmosphere. Although sweep gas regeneration is under investigation, the feasibility, logistics penalties, and failure modes associated with this technique have not been fully determined. TDA Research, Inc. is developing a durable, high-capacity regenerable adsorbent that can remove CO2 from the space suit ventilation loop. The system design allows sorbent regeneration at or above 6 torr, eliminating the potential for Martian atmosphere to leak into the regeneration bed and into the ventilation loop. Regeneration during EVA eliminates the consumable requirement related to the use of LiOH canisters and the mission duration limitations imposed by MetOx system. The concept minimizes the amount of consumable to be brought from Earth and makes the mission more affordable, while providing great operational flexibility during EVA. The feasibility of the concept has been demonstrated in a series of bench-scale experiments and a preliminary system analysis. Results indicate that sorbent regeneration can be accomplished by applying a 14 C temperature swing, while regenerating at 13 torr (well above the Martian atmospheric pressure), withstanding over 1,000 adsorption/regeneration cycles. This paper presents the latest results from these sorbent and system development efforts.

Alptekin, Gokhan↗

NASA NTRS2013

Additional Developments in Atmosphere Revitalization Modeling and Simulation

NASA's Advanced Exploration Systems (AES) program is developing prototype systems, demonstrating key capabilities, and validating operational concepts for future human missions beyond Earth orbit. These forays beyond the confines of earth's gravity will place unprecedented demands on launch systems. They must 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. This paper describes the continuing development of atmosphere revitalization models and simulations in support of the Atmosphere Revitalization Recovery and Environmental Monitoring (ARREM)

Coker, Robert F.↗

NASA NTRS2013

Additional Developments in Atmosphere Revitalization Modeling and Simulation

Coker, Robert F.↗

NASA NTRS2015

Optimization of the Carbon Dioxide Removal Assembly (CDRA-4EU) in Support of the International Space System and Advanced Exploration Systems

The Life Support Systems Project (LSSP) under the Advanced Exploration Systems (AES) program builds upon the work performed under the AES Atmosphere Resource Recovery and Environmental Monitoring (ARREM) project focusing on the numerous technology development areas. The Carbon Dioxide (CO2) removal and associated air drying development efforts are focused on improving the current state-of-the-art system on the International Space Station (ISS) 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. A component of the CO2 removal effort utilizes a virtual Carbon Dioxide Removal Assembly, revision 4 (CDRA-4) test bed to test a large number of potential operational configurations with independent variations in flow rate, cycle time, heater ramp rate, and set point. Initial ground testing will provide prerequisite source data and provide baseline data in support of the virtual CDRA. Once the configurations with the highest performance and lowest power requirements are determined by the virtual CDRA, the results will be confirmed by testing these configurations with the CDRA-4EU ground test hardware. This paper describes the initial ground testing of select configurations. The development of the virtual CDRA under the AES-LSS Project will be discussed in a companion paper.

Knox, James C.↗

NASA NTRS2017

Removal of Carbon Dioxide from Gas Mixtures Using Ion-Exchanged Silicoaluminophosphates

Na+-SAPO-34 sorbents were ion-exchanged with several individual metal cations for CO2 absorption at different temperatures (273-348 K) and pressures (<1 atm). In general, the overall adsorption performance of the exchanged materials increased as follows: Ce3+<Ti3+<Mg2+<Ca2+<Ag+<Na+<Sr2+. The strontium exchanged materials excelled at low-pressure ranges, exhibiting very sharp isotherms slopes at all temperatures. The Sr2+ species were responsible for the surface strong interaction and the cations were occupying exposed sites (SII') in the materials Chabazite cages. All the sorbent materials exhibited higher affinity for CO2 over the other gases tested (i.e., CH4, H2, N2 and O2) due to strong ion-quadrupole interactions. Sr2+-SAPO-34 sorbents are by far the best option for CO2 removal from CH4 mixtures, especially at low concentrations.

Hernandez-Maldonado, Arturo J↗

NASA NTRS2017

Development of Trace Contaminant Control Prototypes for the Primary Life Support System (PLSS)

Results are presented on the development of Trace Contaminant Control (TCC) Prototypes for use in Extravehicular Activities (EVAs), and more specifically in the Primary Life Support System (PLSS). The current TC-control technology involves the use of a packed bed of acid-impregnated granular charcoal, which is non-regenerable, and the carbon-based sorbent under development in this project can be regenerated by exposure to vacuum at room temperature. Data on sorption and desorption of ammonia and formaldehyde, which are major TCs of concern, as well as pressure-drop calculations were used to design and test 1/6-scale and full-scale trace contaminant control system (TCCS) prototypes. Carbon sorbents were fabricated in both the granular and foam-supported forms. Sorbent performance was tested for ammonia sorption and vacuum regeneration in 1/6-scale, and pressure-drop characteristics were measured at flow rates relevant to the PLSS application.

Wojtowicz, Marek↗