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NASA NTRS1992

Spectral identification of chemisorbed CO2 and application to Mars analog materials

The goal of this work is to identify the spectral signature of chemisorbed CO2, to test the efficacy of carbonate formation on Mars-analog materials via CO2 chemisorption, and to identify the surface-chemical characteristics of good chemisorbents, with the intent of assessing the possible geochemical importance of CO2 chemisorption as a quasipermanent CO2 sink in the Martian environment. Our approach is to search for infrared spectral bands that result from chemisorption of CO2 molecules onto chemical reagents and Mars-analog materials, and to identify the salient differences in adsorbents that favor strong, permanent CO2 chemisorption. The total amount of CO2 in the early Martian atmosphere, and consequent surface temperatures, are unknown. A CO2 greenhouse may not have been an adequate mechanism under any circumstances; however, it if were, then most of that CO2 must still be in the near-surface environment; no escape mechanism that could remove it after the decline of channeling has been identified. The only plausible reservoir is carbonate, and there are various remote sensing techniques that can be used to search for it. We are investigating CO2 chemisorption as a permanent CO2 sink, and to aid in interpretation of remotely sensed IR spectra of Mars. A common effect reported in CO2 adsorption studies is the formation of a layer of carbonate or bicarbonate anions on adsorbents that have OH- groups available on their surfaces. Inorganic hydroxyls occur on phyllosilicates, amorphous silicates, metal oxides and hydroxides; it is the most abundant and reactive surface functional group on the surfaces of terrestrial silicates. The process responsible for the reaction is chemisorption. Chemisorption is distinguished from physical adsorption in that there is a transfer of electrons between species, and the formation of a chemical bond. The heat of chemisorption is typically of the same order as heats of chemical reaction (i.e., a few hundred to a few thousand kJ/mole), as opposed to heats of physical adsorption (a few kJ per mole). Chemisorption is an activated process that is promoted by an increase in temperature - quite the opposite of physical adsorption. Chemisorption is not reversible in the sense that physical adsorption is.

Zent, A. P.↗

NASA NTRSDate not supplied

Rapid Cycle Amine 4.0 System Development

Carbon dioxide (CO2) and humidity control is a key function of the spacesuit Portable Life Support Subsystem (PLSS). The latest spacesuit design utilizes a pressure swing bed containing a solid amine sorbent to scrub CO2 and humidity produced by the crewmember from the ventilation loop. The solid amine sorbent removes CO2 and humidity from the ventilation loop through a chemisorption mechanism. Simultaneously, CO2 and humidity are desorbed to vacuum via the two-bed pressure swing system during operation. This continuous regeneration allows for longer Extravehicular Activity (EVA) times while minimizing maintenance, consumables, and power usage. This concept has been in development for over 20 years, during which many prototypes and design iterations have been fabricated and evaluated. This paper discusses the recent Rapid Cycle Amine (RCA) design, development, and testing that has been done to advance the technology. The most recent fabrication is the RCA 3.0. It was delivered to NASA Johnson Space Center in 2015 and has since been tested at the component level and at the integrated PLSS level. The purpose of the component level testing was to understand CO2 removal capacity, end-of-life performance, and establish a baseline performance prior to integrated testing. The RCA 3.0 was integrated into the Exploration Extravehicular Mobility Unit (xEMU) PLSS for a comprehensive Design Verification Test (DVT) series. The integrated testing provided the benefit of characterizing the impact performance degradation has on the system. Many of the RCA requirements were developed through analysis, based on the limitations of the PLSS and, in some cases, assumptions about the system and flow behavior. Integrated testing was an opportunity to validate those requirements and assumptions. While the RCA 3.0 was being tested, the next design iteration, RCA 4.0, was under development. The RCA 4.0 preliminary design phase began in late-2019 and shortly after the Preliminary Design Review, the critical design phase began in 2021. The design work has concluded with the completion of a Pre-Manufacturing Review in 2022. This paper provides an overview of the RCA 4.0 system design, summarizes the results of integrated RCA 3.0 testing, and discusses the pertinence of driving requirements such as mass, volume, and power consumption.

Kelsey Bloom↗

NASA NTRS1993

Spectral analysis of chemisorbed CO2 on Mars analog materials

The goal of this work is to estimate the mass of CO2 that may have been removed to a quasi-stable reservoir on the Martian surface by chemisorption and to estimate the spectral effects of chemisorbed CO2 in remotely-sensed Martian spectra. Our approach is to characterize the conditions most favorable for the formation of carbonate on common terrestrial oxide minerals and to search for infrared spectral bands that result from chemisorption of CO2 molecules onto oxide and other Mars analog materials.

Zent, A. P.↗

NASA NTRS2016

Design and Development Comparison of Rapid Cycle Amine 1.0, 2.0, and 3.0

The development of the Rapid Cycle Amine (RCA) swing-bed technology for carbon dioxide (CO2) removal has been in progress since favorable results were published in 1996. Shortly thereafter, a prototype was designed, developed, and tested successfully and delivered to Johnson Space Center in 1999. An improved prototype was delivered to NASA in 2006 and was notated as RCA 1.0 and sized for the extravehicular activity (EVA). The new RCA swing-bed technology is a regenerative system which employs two alternating solid-amine sorbent beds to remove CO2 and water. The two- bed design employs a chemisorption process whereby the beds alternate between adsorbtion and desorbsion. This process provides for an efficient operation of the RCA so that while one bed is in adsorb (uptake) mode, the other is in the desorb (regeneration) mode. The RCA has now progressed through several iterations of technology readiness levels. Test articles have now been designed, developed, and tested for the advanced space suit portable life support system (PLSS) including RCA 1.0, RCA 2.0, and RCA 3.0. The RCA 3.0 was the most recent RCA fabrication and was delivered to NASA-JSC in June 2015. The RCA 1.0 test article was designed with a pneumatically actuated linear motion spool valve. The RCA 2.0 and 3.0 test articles were designed with a valve assembly which allows for switching between uptake and regeneration modes while minimizing gas volume losses to the vacuum source. RCA 2.0 and 3.0 also include an embedded controller design to control RCA operation and provide the capability of interfacing with various sensors and other ventilation loop components. The RCA technology is low power, small, and has fulfilled all test requirements levied upon the technology during development testing thus far. This paper will provide an overreview of the design and development of RCA 1.0, 2.0 and 3.0 including detail differences between the design specifications of each.

Chullen, Cinda↗

NASA NTRS2016

Design and Development Comparison of Rapid Cycle Amine 1.0, 2.0, and 3.0

The development of the Rapid Cycle Amine (RCA) swing-bed technology for carbon dioxide (CO2) removal has been in progress since favorable results were published in 1996. Shortly thereafter, a prototype was designed, developed, and tested successfully and delivered to Johnson Space Center in 1999. An improved prototype (RCA 1.0) was delivered to NASA in 2006 and sized for the extravehicular activity (EVA). The RCA swing-bed technology is a regenerative system which employs two alternating solid-amine sorbent beds to remove CO2 and water. The two-bed design employs a chemisorption process whereby the beds alternate between adsorption and desorption. This process provides for an efficient RCA operation that enables one bed to be in adsorb (uptake) mode, while the other is in the desorb (regeneration) mode. The RCA has progressed through several iterations of technology readiness levels. Test articles have now been designed, developed, and tested for the advanced space suit portable life support system (PLSS) including RCA 1.0, RCA 2.0, and RCA 3.0. The RCA 3.0 was the most recent RCA fabrication and was delivered to NASA-JSC in June 2015. The RCA 1.0 test article was designed with a pneumatically actuated linear motion spool valve. The RCA 2.0 and 3.0 test articles were designed with a valve assembly which allows for switching between uptake and regeneration modes while minimizing gas volume losses to the vacuum source. RCA 2.0 and 3.0 also include an embedded controller design to control RCA operation and provide the capability of interfacing with various sensors and other ventilation loop components. The RCA technology is low power, small, and has fulfilled all test requirements levied upon the technology during development testing thus far. This paper will provide an overview of the design and development of RCA 1.0, 2.0 and 3.0 including detail differences between the design specifications of each. Nomenclature.

Chullen, Cinda↗

NASA NTRS1990

Chemisorption studies of Pt/SnO2 catalysts

The low temperature CO oxidation catalysts that are being developed and tested at NASA-Langley are fairly unique in their ability to efficiently oxidize CO at low temperatures (approx. 303 K). The bulk of the reaction data that has been collected in the laboratory has been determined using plug flow reactors with a low mass of Pt/SnO2/SiO2 catalyst (approx. 0.1 g) and a modest flow rate (5 to 10 sc sm). The researchers have previously characterized the surface solely in terms of N2 BET surface areas. These surface areas have not been that indicative of reaction rate. Indeed, some of the formulations with high BET surface area have yielded lower reaction rates than those with lower BET surface areas. As a result researchers began a program of determining the chemisorption of the various species involved in the reaction; CO, O2 and CO2. Such a determination of will lead to a better understanding of the mechanism and overall kinetics of the reaction. The pulsed-reactor technique, initially described by Freel, is used to determine the amount of a particular molecule that is adsorbed on the catalyst. Since there is some reaction of CO with the surface to produce CO2, the pulsed reactor had to be coupled with a gas chromatograph in order to distinguish between the loss of CO that is due to adsorption by the surface and the loss that is due to reaction with the surface.

Brown, Kenneth G.↗

NASA NTRS1995

Interstellar Grain Surface Chemistry

Chemistry on grain surfaces plays an Important role in the formation of interstellar Ices, It can also influence the composition of the gas phase through outgassing near luminous, newly formed stars. This paper reviews the chemical processes taking place on Interstellar grain surfaces with the emphasis on those transforming CO into other hydrocarbons. At low, molecular cloud temperatures (approximately equal to 10K), physisorption processes dominate interstellar grain surface chemistry and GO is largely hydrogenated through reactions with atomic H and oxidized through reactions with atomic O. The former will lead to the formation of H2CO and CH3OH ices, while the latter results in CO2 ice. The observational evidence for these ices in molecular clouds will be discussed. Very close to protostars, the gas and grain temperatures are much higher (approximately equal to 500K) and chemisorption processes, including catalytic surface reactions, becomes important. This will be illustrated based upon our studies of the Fischer-Tropsch Synthesis of CH4 from CO on metallic surfaces. Likely, this process has played an important role in the early solar nebula. Observational consequences will be pointed out.

Tielens, Alexander G. G. M.↗

NASA NTRS1986

Summary Abstract: Vibrations of Ammonia on the Cu (100) Surface

Recently, the TR frequencies for NH3 molecularly adsorbed on Cu(100) have been measured by infrared laser-induced photodesorption using a tunable laser operating in the group frequency range. Additionally, photodesorption, photo-fragmentation, and photoionization has been observed using a CO2 laser in the 10 microns range. In this contribution we report on work in progress where we use quantum chemical methods to analyze the shifts in the NH, frequencies relative to the gas phase upon chemisorption. We also compute the Cu- N stretch vibration, which has been observed experimentally,and the change in the IR intensities associated with chemisorption; this change is insufficient by itself to explain the increased photoionization efficiency observed.

Pettersson, Lars G. M.↗

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↗

NASA NTRS1990

Phillips CO-oxidation catalyts for long-lived CO2 lasers: Activity and initial characterization studies

Four different catalysts have been developed specifically for use in sealed carbon dioxide lasers. The catalysts have been designed to be low dusting, stable to shock and vibration, have high activity at low temperatures and have long active lifetimes. Measured global CO oxidation rates range from 1.4 to 2.2 cc CO converted per minute per gram of catalyst at ambient temperature. The catalysts also retain substantial activity at temperatures as low as -35 C. The Phillips laser catalysts are prepared in a variety of different shapes to meet the different pressure drop and gas flow profiles present in the many different styles of lasers. Each catalyst has been tested in sealed TEA lasers and has been shown to substantially increase the sealed life of the laser. Activity measurements made on the precious metal catalysts which were prepared with and without activity promoters showed that the promoter materials increase catalyst CO oxidation activity at least an order of magnitude at ambient temperature. Initial studies using H2 and CO chemisorption, X ray diffraction (XRD) and X ray photoelectron spectroscopy (XPS) have shown that the activity promoters do not significantly affect the precious metal crystallite size or the electronic structure around the precious metal. In addition, the formation or lack of formation of solid solutions between the precious metal and promoters has also been shown not to affect the activity of the promoted catalyst.

Kolts, J. H.↗

NASA NTRS2014

Evaluating the Adsorptive Capabilites of Chemsorb 1000 and Chemsorb 1425

The removal of trace contaminants from spacecraft cabin air is necessary for crew health and comfort during long duration space exploration missions. The air revitalization technologies used in these future exploration missions will evolve from current ISS ISS State-of-Art (SOA) and is being designed and tested by the Advanced Exploration Systems (AES) Program's Atmosphere Resource Recovery and Environmental Monitoring (ARREM) project. The ARREM project is working to mature optimum atmosphere revitalization and environmental monitoring system architectures to enable exploration beyond Lower Earth Orbit (LEO). The Air Revitalization Lab at KSC is one of six NASA field centers participating in the ARREM that specializes in adsorbent and catalyst characterization with simulated spacecraft gas streams using combinations of pressure, O2 partial pressure, CO2 partial pressure, and humidity that are representative of a range of anticipated cabin atmospheric conditions and loads. On board ISS, the Trace Contaminant Control Subassembly (TCCS) provides active control of trace contaminants from the cabin atmosphere utilizing physical adsorption, thermal catalytic oxidation, and chemical adsorption processes. High molecular weight contaminants and ammonia (NH3) are removed a granular activated carbon treated with approx. 10% by weight phosphoric acid (H3PO4) (B-S Type 3032 4×6 mesh), which is expendable and is periodically refurbished. The Type 3032 granular activated carbon bed is no longer commercially available and therefore it is important to characterize the efficiency and capacity of commercially available NH3 sorbents. This paper describes the characterization of two Molecular Products LTD activated carbons: Chemsorb 1000 and Chemsorb 1425. Untreated activated carbons (e.g. Chemsorb 1000) remove contaminants by physisorption, which concentrates the contaminant within the pores of the carbon while letting air to pass through the sorbent4. Low molecular weight or polar gases (e.g. HCl, SO2, formaldehyde, and NH3) are not removed by physisorption and typically require chemisorption for removal. Treated activated carbons (e.g. Chemsorb 1425) are impregnated with a a chemical agent (e.g. phosphoric acid) that reacts with those gases, converting them to solids or salts within the carbon and removes them from the air stream. This process occurs via neutralization or catalysis reactions and adsorption capacity is exhaustedwhen the available impregnated chemicals are consumed. Moisture affects removal performance since adsorption sites within the pores are filled with water. The performance of impregnated carbons may be enhanced by moisture content because the mechanisms of contaminant removal are chemical reactions that occur in reagents contained within the pores. The adsorptive capacity data (mol/kg) of Chemsorb 1000 and 1425 for gas mixtures (ethanol, acetone, toluene, acetaldehyde, dichloromethane, and xylene) was measured with 40% relative humidity at 23 deg C air temperature. The adsorptive capacity data (mol/kg) of Chemsorb 1425 was measured using NH3 gas streams.

adsorptive capacities↗