Search NASA⌕ Search

SEARCH · Search NASA

Results for “limited CO2 activation”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

An integrated experimental–modeling approach to identify key processes for carbon mineralization in fractured mafic and ultramafic rocks

Abstract Controlling atmospheric warming requires immediate reduction of carbon dioxide (CO2) emissions, as well as the active removal and sequestration of CO2 from current point sources. One promising proposed strategy to reduce atmospheric CO2 levels is geologic carbon sequestration (GCS), where CO2 is injected into the subsurface and reacts with the formation to precipitate carbonate minerals. Rapid mineralization has recently been reported for field tests in mafic and ultramafic rocks. However, unlike saline aquifers and depleted oil and gas reservoirs historically considered for GCS, these formations can have extremely low porosities and permeabilities, limiting storage volumes and reactive mineral surfaces to the preexisting fracture network. As a result, coupling between geochemical interactions and the fracture network evolution is a critical component of long-term, sustainable carbon storage. In this paper, we summarize recent advances in integrating experimental and modeling approaches to determine the first-order processes for carbon mineralization in a fractured mafic/ultramafic rock system. We observe the critical role of fracture aperture, flow, and surface characteristics in controlling the quantity, identity, and morphology of secondary precipitates and present where the influence of these factors can be reflected in newly developed thermo-hydro-mechanical–chemical models. Our findings provide a roadmap for future work on carbon mineralization, as we present the most important system components and key challenges that we are overcoming to enable GCS in mafic and ultramafic rocks.

58 GEOSCIENCES↗
DOE OSTI2023

Earth Sciences Applications for Energy and Global Security: A Few Vignettes [Slides]

Understanding the physics of flow and transport in the subsurface environment is crucial to several National Security applications. In the Energy Security realm, some examples include characterizing radioactive waste disposal, exploring natural gas extraction and sequestering CO2. An example in the Global Security arena is to be able to distinguish between anthropogenic and naturally occurring seismic disturbances, the former being of particular concern as underground nuclear testing activity has seen an increase in recent years. A common theme across these applications is the ability to accurately model fluid flow in porous and/or fractured subsurface media. For decades, researchers have grappled with how to include the effects of uncertainties in these models, including but not limited to heterogeneity, unknown initial and boundary conditions and issues with scalability. More recently advances in computing and machine learning methodologies have allowed a broader exploration of the uncertainty space as we strive for real time decision making. I will present an overview of the field and discuss a few examples of how my own research in these topics has evolved over nearly two decades.

58 GEOSCIENCES↗
NASA NTRS2007

Development of a Rapid Cycling CO(sub 2) and H(sub 2)O Removal Sorbent

The National Aeronautics and Space Administration (NASA) planned future missions set stringent demands on the design of the Portable Life Support System (PLSS), requiring dramatic reductions in weight, decreased reliance on supplies and greater flexibility on the types of missions. Use of regenerable systems that reduce weight and volume of the Extravehicular Mobility Unit (EMU) is of critical importance to NASA, both for low orbit operations and for long duration manned missions. The carbon dioxide and humidity control unit in the existing PLSS design is relatively large, since it has to remove and store 8 hours worth of CO2. If the sorbent regeneration can be carried out during the extravehicular activity (EVA) with a relatively high regeneration frequency, the size of the sorbent canister and weight can be significantly reduced. The progress of regenerable CO2 and humidity control is leading us towards the use of a rapid cycling amine system. TDA Research, Inc. is developing compact, regenerable sorbent materials to control CO2 and humidity in the space suit ventilation loop. The sorbent can be regenerated using space vacuum during the EVA, eliminating all carbon dioxide and humidity duration-limiting elements in the life support system. The material also has applications in other areas of space exploration such as the Orion spacecraft and other longer duration exploration missions requiring regenerable technologies. This paper summarizes the results of the sorbent development, testing, and evaluation efforts to date. The results of a preliminary system analysis are also included, showing the size and volume reductions for PLSS provided by the new system.

Paul, Heather↗
DOE OSTI2022

Monitoring Carbon Storage Sites with Time-Lapse Gravity Surveys

Monitoring technologies are deployed on carbon storage sites to demonstrate that the injected CO2 is contained within the storage complex during and long after the active life of the project and that the CO2 behavior is conforming to expectations. Detection of gravity variations accompanying mass redistributions in the subsurface caused by fluid movements in reservoirs provides a unique means for monitoring the dynamics of a carbon sequestration site. Time-lapse gravity surveys have a long history of effectively monitoring temporal density changes in the subsurface. However, monitoring of carbon storage sites with time-lapse gravity surveys using surface or borehole measurements remains limited, although it gained more attention during the last decade. With the recent progresses in instrument capabilities, and the increased number of fluid storage sites (e.g., wastewater, CO2, natural gas, etc.), the gravity method (with its unique ability to remotely estimate both the mass of an injected fluid and its location) has a promising future in monitoring. This chapter provides background information regarding the gravity method and discusses its modeling and application to various carbon storage sites.

Carbon Sequestration, time-lapse gravity, monitori↗
DOE OSTI2022

Linear relationships for modeling CO 2 absorption in aqueous alkanolamine solutions in a thermodynamically consistent way

A thermodynamically consistent model for the carbon dioxide (CO 2 ) absorption in aqueous alkanolamine system is of great importance in the research and development of a CO 2 capture process. To facilitate the development of thermodynamic models, linear Gibbs free energy, enthalpy, and heat capacity relationships using well-known amines as reference are used to correlate the standard reference state properties of ionic species with those of molecular species in the electrolyte system, which has been approved to provide a reliable and consistent way to estimate required parameters when there is minimal or no appropriate experimental data available. Here, the proposed relationships have been applied to the development of an electrolyte nonrandom two liquid (NRTL) activity coefficient model for CO 2 absorption in aqueous 1-amino-2-propanol (A2P) solution, as an example to demonstration the methodology. With limited vapor–liquid equilibrium data and other thermodynamic properties, the parameters in the electrolyte NRTL model are identified with good accuracy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Multiscale Assessment of Caprock Integrity for Geologic Carbon Storage in the Pennsylvanian Farnsworth Unit, Texas, USA

Leakage pathways through caprock lithologies for underground storage of CO2 and/or enhanced oil recovery (EOR) include intrusion into nano-pore mudstones, flow within fractures and faults, and larger-scale sedimentary heterogeneity (e.g., stacked channel deposits). To assess multiscale sealing integrity of the caprock system that overlies the Morrow B sandstone reservoir, Farnsworth Unit (FWU), Texas, USA, we combine pore-to-core observations, laboratory testing, well logging results, and noble gas analysis. A cluster analysis combining gamma ray, compressional slowness, and other logs was combined with caliper responses and triaxial rock mechanics testing to define eleven lithologic classes across the upper Morrow shale and Thirteen Finger limestone caprock units, with estimations of dynamic elastic moduli and fracture breakdown pressures (minimum horizontal stress gradients) for each class. Mercury porosimetry determinations of CO2 column heights in sealing formations yield values exceeding reservoir height. Noble gas profiles provide a “geologic time-integrated” assessment of fluid flow across the reservoir-caprock system, with Morrow B reservoir measurements consistent with decades-long EOR water-flooding, and upper Morrow shale and lower Thirteen Finger limestone values being consistent with long-term geohydrologic isolation. Together, these data suggest an excellent sealing capacity for the FWU and provide limits for injection pressure increases accompanying carbon storage activities.

58 GEOSCIENCES↗
DOE OSTI2022

Making Grid-interactive Efficient Buildings a “Win” for Both Customers and Utilities

Buildings account for more than 70% of U.S. electricity use and at least one-third of U.S. economy-wide CO2 emissions. Changing the timing and overall amount of electricity consumption in buildings would significantly reduce energy costs to consumers and facilitate the transition to a decarbonized economy. Grid-interactive efficient buildings (GEBs) incorporate energy efficiency, smart technologies, and active use of distributed energy resources (DERs) to provide these benefits. As the link between the customer and the power system, utilities are central to widespread deployment of GEBs. Yet, despite the significant cost savings and operational benefits of GEBs for utilities, deployment has remained limited. This paper explores emerging models for enabling utilities to facilitate GEB adoption. Building off foundational research conducted to develop the U.S. DOE’s A National Roadmap for Grid-Interactive Efficient Buildings, we describe the most novel recent examples of ways in which utilities and regulators have made demand-side innovation a win for both the customer and the utility. Emerging concepts include: (1) performance incentive mechanisms to align GEB deployment with utility financial motivations, (2) the use of subscription pricing (i.e., fixed monthly bills) to promote load flexibility and energy efficiency, (3) rate-basing utility-controlled behind-the-meter assets, and (4) coupling energy efficiency and load flexibility with electrification proposals to ensure that customer benefits are maximized. The paper concludes with a discussion about prospects for widespread GEB deployment and utilization by utilities, and how to scale efforts.

Satchwell, Andrew↗
DOE OSTI2022

Kinetics and Reactor Modeling of VFA Ketonization for Sustainable Aviation Fuel Production

Ketonization of volatile fatty acids (VFAs) produced via arrested methanogenesis of wet waste represents the only unit operation of wet waste upgrading to sustainable (net-zero or negative life cycle CO2 emissions) aviation fuel not currently in industrial practice. Ketone product yields of close to 100% have been obtained during gas-phase reactions of VFAs over oxide catalysts at the laboratory scale, but design of an industrial ketonization reactor requires understanding of the impacts of reactant and product partial pressures, deactivation, and heat and mass transport phenomena on observed ketonization rates. Our work leverages rigorous kinetic analysis of ketonization processes to inform reactor scale-up efforts through packed-bed reactor modeling. We first present results of a kinetic study of ketonization of a model VFA, hexanoic acid, over an industrial ZrO2 catalyst performed in a packed-bed microreactor in conditions free of significant heat or mass transfer gradients. Major findings of the analysis include: (i) hexanoic acid saturates all catalyst active sites at relatively low partial pressure (~10 kPa) and (ii) ketonization products 6-undecanone, water, and CO2 inhibit reaction rates. Kinetic data are used to fit a rate expression quantifying the functional dependence of ketonization rate on partial pressures of VFA reactants and ketone, water, and CO2 products. A packed-bed reactor model describing vapor-phase hexanoic acid ketonization over ZrO2 extrudate catalysts is developed based on the kinetic model. The effects of (i) bed- and pellet-scale mass- and heat-transfer limitations and (ii) axial pressure drop guide our development of recommendations for optimal sizing, temperature, and influent flow composition of an industrial-scale ketonization reactor. The quantitative understanding of VFA ketonization developed in this study represents an advance toward derisking the VFA ketonization step of wet waste upgrading to sustainable aviation fuel.

biojet↗
NASA NTRS1989

C-O-H ratios of silicate melt inclusions in basalts from the Galapagos Spreading Center near 95 degrees W: a laser decrepitation mass spectrometry study

Volatile ratios (primarily of H2O and CO2) in individual silicate melt (glass) inclusions in minerals have been analyzed using laser volatilization and mass spectrometry. A Nd-glass laser was used to produce 50-micrometer diameter pits in silicate melt inclusions. Released volatiles were analyzed directly with a computer-controlled quadrupole mass spectrometer. The detection limits for CO2 and H2O were on the order of 3 x 10(-14) and 3 x 10(-13) moles, respectively. The reproducibility for CO2/H2O was better than +/- 9%. The total range of volatile ratios from vitreous silicate glass inclusions contained in a suite of Galapagos lavas were: 0.018 to 1.193 for CO2/H2O; 0.002 to 0.758 for CO/H2O; 0 to 0.454 for CH4/H2O; and 0 to 0.432 for Ar/H2O. The mean CO2/H2O from the propagating rift (0.245 +/- 0.068) silicate glass inclusions is significantly lower than that of the actively failing rift (0.641 +/- 0.241); this difference probably reflects different degrees of degassing during magmatic histories for the two regions. Relatively undifferentiated failing rift magmas must have relatively short crustal residence times prior to eruption and, therefore, have not undergone significant degassing of CO2, as would appear to be the case for the more highly fractionated propagating rift magmas. The laser-mass spectrometric system described herein has the ability to act as a point-source probing device that can differentiate between the various volatile sites in minerals and rocks (as well as synthetic materials) on a micrometer scale.

NASA Discipline Exobiology↗
DOE OSTI2024

Experimental Combustion and Flame Characterization of a Chemical Looping-Based Oxidative Dehydrogenation Byproduct Fuel Mixture Containing High CO2 Dilution

Abstract This study investigates the combustion performance of a CO2-rich fuel mixture containing ethane and methane as active species using a constant volume combustion chamber. This fuel is obtained as a byproduct of a chemical looping-based oxidative dehydrogenation (Cl-ODH) process ethylene production. The byproduct gas mixture has 40.79% CO2, 39.49% ethane, and 4.88% methane by weight with other minor compounds. Using this fuel for energy extraction would improve the process efficiency of the ethane to ethylene conversion. After initial combustion modeling, the gas fuel mixture was reduced to just the major species: CO2, ethane, and methane. The mixture was then tested for flammability limits and combustion performance under spark-ignition conditions. Effects of ambient conditions like temperatures between 300 and 400 K with initial pressures from 1 to 10 bar were tested. The effects of stoichiometry were tested to understand flame velocities and heat release. The fuel mixture showed an overall reduced flame velocity compared to gasoline. Instability in combustion was believed to be caused by the dissociation of ethane under elevated conditions. At higher pressures, the flame produces lower cumulative heat release. Simulations were also performed using a model tuned to replicate the operations of the combustion chamber used in the experiments. Heat release and unburnt fuel mass data were calculated to identify the discrepancies in the combustion completeness at elevated pressures. The effects of CO2 quenching the flame coupled with the increased dissociation of the fuel species can lead to up to more than 75% of the fuel mixture being unburnt. Data from this study were used to modify a small-scale spark-ignition engine to use this fuel and produce usable energy.

Energy & Fuels↗
NASA NTRS1990

CO-oxidation catalysts: Low-temperature CO oxidation over Noble-Metal Reducible Oxide (NMRO) catalysts

Oxidation of CO to CO2 is an important reaction technologically and environmentally and a complex and interesting reaction scientifically. In most cases, the reaction is carried out in order to remove CO as an environmental hazard. A major application of heterogeneous catalysts is catalytic oxidation of CO in the exhaust of combustion devices. The reaction over catalysts in exhaust gas is fast and often mass-transfer-limited since exhaust gases are hot and O2/CO ratios are high. The main challenges to catalyst designers are to control thermal sintering and chemical poisoning of the active materials. The effect of the noble metal on the oxide is discussed, followed by the effect of the oxide on the noble metal, the interaction of the noble metal and oxide to form unique catalytic sites, and the possible ways in which the CO oxidation reaction is catalyzed by the NMRO materials.

Herz, Richard K.↗
NASA NTRS2012

Miniaturized Laser Heterodyne Radiometer (LHR) for Measurements of Greenhouse Gases in the Atmospheric Column

This passive laser heterodyne radiometer (LHR) instrument simultaneously measures multiple trace gases in the atmospheric column including carbon dioxide (CO2) and methane (CH4), and resolves their concentrations at different altitudes. This instrument has been designed to operate in tandem with the passive aerosol sensor currently used in AERONET (an established network of more than 450 ground aerosol monitoring instruments worldwide). Because aerosols induce a radiative effect that influences terrestrial carbon exchange, simultaneous detection of aerosols with these key carbon cycle gases offers a uniquely comprehensive measurement approach. Laser heterodyne radiometry is a technique for detecting weak signals that was adapted from radio receiver technology. In a radio receiver, a weak input signal from a radio antenna is mixed with a stronger local oscillator signal. The mixed signal (beat note, or intermediate frequency) has a frequency equal to the difference between the input signal and the local oscillator. The intermediate frequency is amplified and sent to a detector that extracts the audio from the signal. In the LHR instrument described here, sunlight that has undergone absorption by the trace gas is mixed with laser light at a frequency matched to a trace gas absorption feature in the infrared (IR). Mixing results in a beat signal in the RF (radio frequency) region that can be related to the atmospheric concentration. For a one-second integration, the estimated column sensitivities are 0.1 ppmv for CO2, and <1 ppbv for CH4. In addition to producing a standalone ground measurement product, this instrument could be used to calibrate/validate four Earth observing missions: ASCENDS (Active Sensing of CO2 Emissions over Nights, Days, and Seasons), OCO-2 (Orbiting Carbon Observatory), OCO-3, and GOSAT (Greenhouse gases Observational SATellite). The only network that currently measures CO2 and CH4 in the atmospheric column is TCCON (Total Carbon Column Observing Network), and only two of its 16 operational sites are in the United States. TCCON data is used for validation of GOSAT data, and will be used for OCO-2 validation. While these Fourier-transform spectrometers (FTS) can measure the largest range of trace gases, the network is severely limited due to the high cost and extreme size of these instruments (these occupy small buildings and require personnel for operation). The LHR/AERONET instrument offers a significantly smaller (carry-on luggage size) autonomous instrument that can be incorporated into AERONET s much larger (450 instruments) global network.

Steel, Emily↗
NASA NTRS1990

Definition of experiments to investigate fire suppressants in microgravity

Defined and justified here are the conceptual design and operation of a critical set of experiments expected to yield information on suppressants and on suppressant delivery systems under realistic spacecraft-fire conditions (smoldering). Specific experiment parameters are provided on the solid fuel (carbon), oxidants (habitable spacecraft atmospheres), fuel/oxidant supply, mixing mode, and rate (quiescent and finite; ventilated and replenishable), ignition mode, event, and reignition tendency, fire-zone size, fire conditions, lifetime, and consequences (toxicity), suppressants (CO2, H2O, N2) and suppressant delivery systems, and diagnostics. Candidate suppressants were identified after an analysis of how reduced gravity alters combustion, and how these alterations may influence the modes, mechanisms, and capacities of terrestrial agents to suppress unwanted combustion, or fire. Preferred spacecraft suppression concepts included the local, near-quiescent application of a gas, vapor, or mist that has thermophysical fire-suppression activity and is chemically inert under terrestrial (normal gravity) combustion conditions. The scale, number, and duration (about 1 hour) of the proposed low-gravity experiments were estimated using data not only on the limitations imposed by spacecraft-carrier (Shuttle or Space Station Freedom) accommodations, but also data on the details and experience of standardized smolder-suppression experiments at normal gravity. Deliberately incorporated into the conceptual design was sufficient interchangeability for the prototype experimental package to fly either on Shuttle now or Freedom later. This flexibility is provided by the design concept of up to 25 modular fuel canisters within a containment vessel, which permits both integration into existing low-gravity in-space combustion experiments and simultaneous testing of separate experiments to conserve utilities and time.

Reuther, James J.↗
DOE OSTI2025

Fast growth and high-titer bioproduction from renewable formate via metal-dependent formate dehydrogenase in Escherichia coli

Microbial bioproduction using one-carbon (C1) feedstocks has the potential to decarbonize the manufacturing of materials, fuels, and chemicals. Formate is a promising C1 feedstock, and the realization of industrial, formatotrophic platform organisms is a key goal for C1-based bioproduction. So far, a major limitation for synthetic formatotrophy has been slow energy supply due to slow formate dehydrogenase activity. Here, we implement a fast, metal-dependent formate dehydrogenase complex in a synthetic formatotrophic Escherichia coli utilizing the reductive glycine pathway. After a short-term evolution, we demonstrate formatotrophic growth of E. coli with a doubling time of less than 4.5 h, comparable to the fastest natural formatotrophs. To further explore the potential of a formate-based bioeconomy, this strain is engineered to produce mevalonate, as well as the terpenoid and aviation fuel precursor isoprenol, using formate we generate directly from the electrochemical reduction of CO2. This work demonstrates an improvement in bioproduct titer from formate, achieving the production of 3.8 g/L of mevalonate. Additionally, the abundant and recalcitrant polymer lignin is chemically decomposed into a formate-rich mixture of small organic acids and subsequently bioconverted into mevalonate. Overall, the described fast-growing, formatotrophic bioproduction strain demonstrates that a sustainable formate bioeconomy is within reach.

Cowan, Aidan E↗
DOE OSTI2024

Formation of (Rh–Fe)–FeO x Complex Sites Enables Methanol Synthesis from CO 2

Here, we addressed the challenges of designing catalysts for selective CO 2 hydrogenation by incorporating oxide Fe species onto Rh nanoparticles. Nanoscopic FeO x domains created a “reverse catalyst” structure (i.e., a metal oxide supported on a metal) that increased the density of interfacial sites compared to traditional supported catalysts. The contact between the metal nanoparticle and the oxide overlayer induced the formation of a surface Rh-Fe alloy that stabilize methoxy groups while suppressing hydrogenolysis to methane. Sites at FeO x -metal interfaces interact with CO 2 sevenfold stronger than sites on metal surfaces, show larger energy barriers to cleave the C-O bonds, and offer a barrierless pathway for hydrogenation of methoxy species to methanol. Consequently, the multifunctional sites over FeO x /Rh-Fe catalysts highlight and meet the requirements of a selective methanol catalyst: strong interaction with CO 2 to ensure high density of transition states; metal sites to activate and make hydrogen available to surface intermediates; and high energy barriers for C-O bond cleavage to form carbides. These synthesis and catalytic chemistries, demonstrated for Rh-Fe-FeO x interfaces, enable us to overcome the limitations to the design of methanol production catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

A review of in situ/operando studies of heterogeneous catalytic hydrogenation of CO 2 to methanol

Repurposing CO 2 into chemicals, one of the Carbon Dioxide Removal (CDR) strategies, still faces significant challenges in conversion and energy efficiency due to the lack of effective catalysts and processes. Fundamental understanding through in situ/operando investigations of the reaction mechanisms and catalyst structures is pivotal for developing the efficient catalysts. This paper reviews the past and recent in situ/operando studies of methanol synthesis from heterogeneous CO 2 hydrogenation over a few typical catalysts including Cu-based, oxide-based, and noble-metal-based catalysts. With the development of high-pressure reactors, in situ/operando IR, X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), neutron diffraction and imaging have been used to reveal the surface intermediates and structures of working catalysts under CO 2 hydrogenation conditions. On the one hand, the combined operando techniques shed light on working mechanisms for some catalytic systems. On the other hand, due to the complexity of selective CO 2 hydrogenation reaction and limited sensitivity of current accessible operando techniques to the surface structure of catalysts, it is still murky about the exact nature of the active sites at the surface/interface and how different sites promote different reaction paths. Furthermore, it is concluded that new methodologies for differentiating signals from different sites, and the development of surface-sensitive techniques for high pressure reactions are needed for providing structural descriptors of highly active and selective CO 2 conversion catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1973

In situ detection of microbial respiration in soils and salt flats

Increase in CO2 partial pressures over a desert soil treated with casamino-acids glucose solution correlated with bacterial growth. Few or no increases in numbers of bacteria or CO2 concentrations were noted in similar plots treated with water only or receiving no treatment. Growth in the soil appeared to be severely nutrient limited during the 10 day experiment. Especially rapid growth took place between the third and fifth day, when temperatures ranged from 0 deg. (night) to a maximum of 17.4 deg. (day). Under the conditions of the experiment, intermittent CO2 assay was an insensitive indicator of growth, possibly because of restiction of gas escape by the desert pavement or solution, exchange, or precipitation of carbonate, but more likely because of inefficient sealing of hoods to and below the soil surface. CO2 assay was unable to detect microbial successions. The unpredictable course of these successions, plus unpredictable relative retentions mitigates against assay of organic gases as reliable in situ detection of microbial activity, except perhaps in very alkaline environments such as Owens Lake salts.

Tew, R. W.↗