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DOE OSTI2025

Reactive Capture and Conversion of Carbon Dioxide to Methanol with ZnZrO 2 and Alkali-Promoted Mg 3 AlO x Mixed Oxide Catalytic Sorbents

Reactive capture and conversion (RCC) explores the use of a single-unit process to capture CO 2 and produce a product, in this case, methanol (MeOH). In this study, different configurations of a catalytic sorbent (CS) composed of ZnZrO 2 catalyst and Mg 3 AlO x sorbent with and without alkali modification are evaluated for CO 2 adsorption, steady-state catalysis with cofed CO 2 and H 2 , and transient RCC performance. A catalyst composed of a physical mixture of Mg 3 AlO x with ZnZrO 2 resulted in a slight increase in CO 2 uptake, with a low impact on the catalytic activity and RCC of the materials compared to ZnZrO 2 alone. In contrast, Na impregnation significantly increased the level of CO 2 uptake from 0.28 mmol/g (ZnZrO 2 alone) to 0.6 and 1.1 mmol/g for the CS with Na on the catalyst or Mg 3 AlO x , respectively. However, Na impregnation reduced the CO 2 conversion rate and MeOH selectivity during steady-state cofeed experiments at 300 °C and 6 bar. In contrast to steady-state catalysis conditions, RCC, which is a cyclic capture and conversion process, creates dynamic CO 2 and H 2 surface coverages, favoring CH 4 in the early stages of the conversion step and then CO and MeOH as the catalyst CO 2 coverage reduces. The highest MeOH productivity during RCC was achieved with CS that balanced the CO 2 uptake with only moderate catalyst rate reductions caused by Na addition. The optimal material, ZnZrO 2 +10%Na/Mg 3 AlO x , achieved a CO 2 uptake of 0.8 mmol/g and a MeOH productivity of 0.5 mmol/g with 100% selectivity at 260 °C and 6 bar during RCC. This marks the highest RCC MeOH productivity reported to date, although the process needs further optimization and even with optimization, may remain impractical. The results further demonstrate that optimization of catalytic sorbents under steady-state flow conditions does not easily correlate to transient capture and conversion cycles for methanol synthesis from CO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRSDate not supplied

Nondestructive Evaluation for the Space Shuttle's Wing Leading Edge

The loss of the Space Shuttle Columbia highlighted concerns about the integrity of the Shuttle's thermal protection system, which includes Reinforced Carbon-Carbon (RCC) on the leading edge. This led NASA to investigate nondestructive evaluation (NDE) methods for certifying the integrity of the Shuttle's wing leading edge. That investigation was performed simultaneously with a large study conducted to understand the impact damage caused by errant debris. Among the many advanced NDE methods investigated for applicability to the RCC material, advanced digital radiography, high resolution computed tomography, thermography, ultrasound, acoustic emission and eddy current systems have demonstrated the maturity and success for application to the Shuttle RCC panels. For the purposes of evaluating the RCC panels while they are installed on the orbiters, thermographic detection incorporating principal component analysis (PCA) and eddy current array scanning systems demonstrated the ability to measure the RCC panels from one side only and to detect several flaw types of concern. These systems were field tested at Kennedy Space Center (KSC) and at several locations where impact testing was being conducted. Another advanced method that NASA has been investigating is an automated acoustic based detection system. Such a system would be based in part on methods developed over the years for acoustic emission testing. Impact sensing has been demonstrated through numerous impact tests on both reinforced carbon-carbon (RCC) leading edge materials as well as Shuttle tile materials on representative aluminum wing structures. A variety of impact materials and conditions have been evaluated including foam, ice, and ablator materials at ascent velocities as well as simulated hypervelocity micrometeoroid and orbital debris impacts. These tests have successfully demonstrated the capability to detect and localize impact events on Shuttle's wing structures. A first generation impact sensing system has been designed for the next Shuttle flight and is undergoing final evaluation for deployment on the Shuttle's first return to flight. This system will employ wireless accelerometer sensors that were qualified for other applications on previous Shuttle flights. These sensors will be deployed on the wing's leading edge to detect impacts on the RCC leading edge panels. The application of these methods will help to insure the continued integrity of the Shuttle wing's leading edge system as the Shuttle flights resume and until their retirement.

Eric I Madaras↗

NASA NTRS2004

Understanding Columbia's Reentry Problems

Soon after the Space Shuttle Columbia accident occurred last year, a group of CFD analysts from NASA centers and private industry was organized to help determine the cause of the accident. This group was under the direction of the Applied Aeroscience and CFD Branch of the Aeroscience and Flight Mechanics Division at the Johnson Space Center. For external flow simulations, noncommercial CFD codes that specialize in hypersonic or high Mach number flows were used. These tools were used to determine heating rates, pressures, and temperatures for a large number of vehicle damage scenarios. Lockheed Martin Space Operations was called upon to provide CFD support in the area of internal flows within the shuttle wing cavity, and or these simulations, FLUENT 6.1 was chosen. Two large-scale, simplified models were run to understand the flow patterns once a breach of the internal wing cavity was initiated. The results were primarily used to visualize flow patterns within the wing cavity. The first CFD model included the entire left wing without the wheel. well cavity. The purpose of the first model, which did not include the reinforced carbon-carbon (RCC) cavity along the wing leading edge, was to visualize the flow field within the wing cavity immediately after the leading edge spar breach, This model assumed that the flow coming into the wing cavity was nom1 to the spar. It included all o f the primary vents that allow for flow between the main cavities of the wing. A six-inch diameter hole was modeled in the spar at the approximate location where the spar breach was judged to have occurred, which was between RCC panels 8 and 9. The results of the modeling showed that at this location, the high temperature, high velocity gas stream entering the wing cavity impinged on the outboard wheel well cavity. Instrumentation in the Shuttle wheel well cavity registered abnormal temperatures during reentry, so the FLUENT results helped support the conclusion of the accident investigation team that the spar breach was in the RCC panel 8-9 area, and that the initial spar breach was likely entering the wing cavity normal to the spar. This model also showed that the flow entering the wing cavity tended to swirl within the cavity just outboard of the wheel well, and did not initially penetrate further into the rear cavities of the wing. The second CFD model was a 2-D simulation of the left wing cavity and the RCC cavity. It was used to visualize the flow through the RCC breach, through the wing spar breach, and into the wing cavity directly outboard of the wheel well. The purpose of this model was to verify whether or not it was possible for the flow to come into the wing cavity normal to the leading edge spar. The results from this 2-D model showed that the internal structure behind the RCC panels probably deflected the flow entering the RCC cavity so that it impinged normal to the spar. As in the 3-D model, this deflected flow stream was found to impinge on the wheel well outer wall. This model again supported the conclusions regarding the location of the spar breach and how the flow behaved inside the wing cavity.

Paul, Thomas H.↗

NASA NTRS2006

Understanding Columbia's Reentry Problems

Soon after the Space Shuttle Columbia accident occurred last year, a group of CFD analysts from NASA centers and private industry was organized to help determine the cause of the accident. This group was under the direction of the Applied Aeroscience and CFD Branch of the Aeroscience and Flight Mechanics Division at the Johnson Space Center. For external flow simulations, noncommercia2 CFD codes that specialize in hypersonic or high Mach number flows were used. These tools were used to determine heating rates, pressures, and temperatures for a large number of vehicle damage scenarios. Lockheed Martin Space Operations was called upon to provide CFD support in the area of internal flows within the shuttle wing cavity, and for these simulations, FLUENT 6.1 was chosen. Two large-scale, simplified models were m to understand the flow patterns once a breach of the internal wing cavity was initiated. The results were primarily used to visualize flow patterns within the wing cavity. The first CFD model included the entire lee wing without the wheel well cavity. The purpose of the first model, which did not include the reinforced carbon-carbon (RCC) cavity along the wing leading edge, was to visualize the flow field within the wing cavity immediately after the leading edge spar breach, This model assumed that the flow coming into the wing cavity was normal to the spar. It included all of the primary vents that allow for flow between the main cavities of the wing. A six-inch diameter hole was modeled in the spar at the approximate location where the spar breach was judged to have occurred, which was between RCC panels 8 and 9. The results of the modeling showed that at this location, the high temperature, high velocity gas stream entering the wing cavity impinged on the outboard wheel well cavity. Instrumentation in the Shuttle wheel well cavity registered abnormal temperatures during reentry, so the FLUENT results helped support the conclusion of the accident investigation team that the spar breach was in the RCC panel 8-9 area, and that the initial spar breach was likely entering the wing cavity normal to the spar. This model also showed that the flow entering the wing cavity tended to swirl within the cavity just outboard of the wheel well, and did not initially penetrate further into the rear cavities of the wing. The second CFD model was a 2-D simulation of the left wing cavity and the RCC cavity. It was used to visualize the flow through the RCC breach, through the wing spar breach, and into the wing cavity directly outboard of the wheel well. The purpose of this model was to verify whether or not it was possible for the flow to come into the wing cavity normal to the leading edge spar. The results from this 2-D model showed that the internal structure behind the RCC panels probably deflected the flow entering the RCC cavity so that it impinged normal to the spar. As in the 3-D model, this deflected flow stream was Found to impinge on the wheel well outer wall. This model again supported the conclusions regarding the location of the spar breach and how the flow behaved inside the wing cavity.

Paul, Thomas↗

DOE OSTI2025

Comparative techno-economic analysis of synthetic renewable natural gas production via reactive CO 2 capture and conversion

Reactive CO 2 capture and conversion (RCC) is an emerging carbon management strategy that integrates CO 2 capture and conversion and avoids intermediate CO 2 purification. In this study, we design an RCC process to capture atmospheric CO 2 and react it with renewable hydrogen to produce synthetic renewable natural gas (SRNG), which serves as a carbon-neutral energy source and a chemical form of long-duration renewable energy storage. We assess the technological potential of RCC through process modeling, techno-economic, carbon footprint, and sensitivity analyses. Our findings demonstrate that RCC offers energy savings and comparable cost to separated capture and conversion processes. The cost is dominated by renewable hydrogen and material replacement cost. SRNG produced via RCC is competitive with existing low-carbon natural gas technologies and presents a promising low-cost option for long-duration energy storage. This work highlights the potential for deploying RCC technologies within a circular carbon economy and the scientific and technical challenges that must be overcome for material and technology developers.

03 NATURAL GAS↗

DOE OSTI2025

Cation Effects on CO 2 Delivery to Cu Electrode in Reactive Capture of CO 2

The direct electrochemical conversion of captured CO 2 , known as reactive capture of CO 2 (RCC), remains a formidable challenge in heterogeneous catalysis. Given that amines are one of the most widely used capture agents for CO 2 , it would be desirable to electrochemically reduce the resultant adducts, such as carbamate, directly in RCC. However, current understanding suggests that the primary species undergoing reduction in RCC with amines is the CO 2 dissociated from the sorbent. Herein, we employ ab initio molecular dynamics (AIMD) with DFT to analyze how the nature of alkali metal cations in the electrolyte affects carbamate at the Cu surface, thereby assessing the possibility of promoting RCC by cation effects. The simulations show that the carbamate’s orientation with respect to the electrode is governed by the optimal distance between the carbamate and the cation, specifically how this distance aligns with the cation’s hydration spheres. Moreover, the slow-growth AIMD results indicate that the CO 2 dissociation barrier correlates with the orientation of carbamate at the interface. When the carbamate resides beyond the cation’s first hydration sphere, it adopts a flat orientation with respect to the surface that promotes the release of CO 2 from the capture agent. In contrast, when the carbamate disrupts the first hydration sphere and exhibits a strong cation−π interaction, it adopts an upright orientation that is less conducive to CO 2 release. These findings reveal a nontrivial cation effect in RCC, suggesting that it should be possible to optimize RCC via the choice of the electrolyte.

ab initio molecular dynamics↗

NASA NTRS1976

Ablative performance of uncoated silicone-modified and shuttle baseline reinforced carbon composites

The relative ablative performance of uncoated silicone-modified reinforced carbon composite (RCC) and uncoated shuttle baseline RCC substrates was investigated. The test specimens were 13 plies (5.3 to 5.8 millimeters) thick and had a 25-millimeter-diameter test face. Prior to arc tunnel testing, all specimens were subjected to a heat treatment simulating the RCC coating process. During arc tunnel testing, the specimens were exposed to cold wall heating rates of 178 to 529 kilowatts/sq m and stagnation pressures ranging from 0.015 to 0.046 atmosphere at Mach 4.6 in air, with and without preheating in nitrogen. The results show that the ablative performance of uncoated silicone-modified RCC substrates is significantly superior to that of uncoated shuttle baseline RCC substrates over the range of heating conditions used. These results indicate that the silicone-modified RCC substrate would yield a substantially greater safety margin in the event of complete coating loss on the shuttle orbiter.

Dicus, D. L.↗

NASA NTRS2000

Oxidation of Reinforced Carbon-Carbon Subjected to Hypervelocity Impact

This paper presents results from arc jet tests conducted at the NASA Johnson Space Center on reinforced carbon-carbon (RCC) samples subjected to hypervelocity impact. The RCC test specimens are representative of RCC components used on the Space Shuttle Orbiter. The arc jet testing established the oxidation characteristics of RCC when hypervelocity projectiles, simulating meteoroid/orbital debris, impact the RCC material. In addition to developing correlations for use in trajectory simulations, we discuss analytical modeling of the increased material oxidation in the impacted area using measured hole growth data. Entry flight simulations are useful in assessing the increased Space Shuttle RCC component degradation as a result of impact damage and the hot gas flow through an enlarging hole into the wing leading-edge cavity.

Curry, Donald M.↗

NASA NTRS2000

Orbiter Reinforced Carbon-Carbon Advanced Sealant Systems: Screening Tests

Oxidation protection for the Orbiter reinforced carbon-carbon (RCC consists of three components: silicon carbide coating, tetraethyl orthosilicate (TEOS) impregnated into the carbon substrate and a silicon based surface sealant (designated Type A). The Orbiter Type A sealant is being consumed each mission, which results in increased carbon-carbon substrate mass loss, which adversely impacts the mission life of the RCC components. In addition, the sealant loss in combination with launch pad contamination (salt deposit and zinc oxide) results in RCC pinholes. A sealant refurbishment schedule to maintain mission life and minimize affects of pin hole formation has been implemented in the Orbiter maintenance schedule. The objective of this investigation is to develop an advanced sealant system for the RCC that extends the refurbishment schedule by reducing sealant loss/pin hole formation and that can be applied to existing Orbiter RCC components. This paper presents the results of arc jet screening tests conducted on several sealants that are being considered for application to the Orbiter RCC.

Curry, Donald M.↗

NASA NTRS2005

Application of Eddy Current Techniques for Orbiter Reinforced Carbon-Carbon Structural Health Monitoring

The development and application of advanced nondestructive evaluation techniques for the Reinforced Carbon-Carbon (RCC) components of the Space Shuttle Orbiter Leading Edge Structural Subsystem (LESS) was identified as a crucial step toward returning the shuttle fleet to service. In order to help meet this requirement, eddy current techniques have been developed for application to RCC components. Eddy current technology has been found to be particularly useful for measuring the protective coating thickness over the reinforced carbon-carbon and for the identification of near surface cracking and voids in the RCC matrix. Testing has been performed on as manufactured and flown RCC components with both actual and fabricated defects representing impact and oxidation damage. Encouraging initial results have led to the development of two separate eddy current systems for in-situ RCC inspections in the orbiter processing facility. Each of these systems has undergone blind validation testing on a full scale leading edge panel, and recently transitioned to Kennedy Space Center to be applied as a part of a comprehensive RCC inspection strategy to be performed in the orbiter processing facility after each shuttle flight.

Wincheski, Buzz↗

NASA NTRS2009

Impact Testing on Reinforced Carbon-Carbon Flat Panels with Ice Projectiles for the Space Shuttle Return to Flight Program

Following the tragedy of the Orbiter Columbia (STS-107) on February 1, 2003, a major effort commenced to develop a better understanding of debris impacts and their effect on the space shuttle subsystems. An initiative to develop and validate physics-based computer models to predict damage from such impacts was a fundamental component of this effort. To develop the models it was necessary to physically characterize reinforced carbon-carbon (RCC) along with ice and foam debris materials, which could shed on ascent and impact the orbiter RCC leading edges. The validated models enabled the launch system community to use the impact analysis software LS-DYNA (Livermore Software Technology Corp.) to predict damage by potential and actual impact events on the orbiter leading edge and nose cap thermal protection systems. Validation of the material models was done through a three-level approach: Level 1--fundamental tests to obtain independent static and dynamic constitutive model properties of materials of interest, Level 2--subcomponent impact tests to provide highly controlled impact test data for the correlation and validation of the models, and Level 3--full-scale orbiter leading-edge impact tests to establish the final level of confidence for the analysis methodology. This report discusses the Level 2 test program conducted in the NASA Glenn Research Center (GRC) Ballistic Impact Laboratory with ice projectile impact tests on flat RCC panels, and presents the data observed. The Level 2 testing consisted of 54 impact tests in the NASA GRC Ballistic Impact Laboratory on 6- by 6-in. and 6- by 12-in. flat plates of RCC and evaluated three types of debris projectiles: Single-crystal, polycrystal, and "soft" ice. These impact tests helped determine the level of damage generated in the RCC flat plates by each projectile and validated the use of the ice and RCC models for use in LS-DYNA.

Melis, Matthew E.↗

NASA NTRS2009

Impact Testing on Reinforced Carbon-Carbon Flat Panels With BX-265 and PDL-1034 External Tank Foam for the Space Shuttle Return to Flight Program

Following the tragedy of the Orbiter Columbia (STS-107) on February 1, 2003, a major effort commenced to develop a better understanding of debris impacts and their effect on the space shuttle subsystems. An initiative to develop and validate physics-based computer models to predict damage from such impacts was a fundamental component of this effort. To develop the models it was necessary to physically characterize reinforced carbon-carbon (RCC) along with ice and foam debris materials, which could shed on ascent and impact the orbiter RCC leading edges. The validated models enabled the launch system community to use the impact analysis software LS-DYNA (Livermore Software Technology Corp.) to predict damage by potential and actual impact events on the orbiter leading edge and nose cap thermal protection systems. Validation of the material models was done through a three-level approach: Level 1-fundamental tests to obtain independent static and dynamic constitutive model properties of materials of interest, Level 2-subcomponent impact tests to provide highly controlled impact test data for the correlation and validation of the models, and Level 3-full-scale orbiter leading-edge impact tests to establish the final level of confidence for the analysis methodology. This report discusses the Level 2 test program conducted in the NASA Glenn Research Center (GRC) Ballistic Impact Laboratory with external tank foam impact tests on flat RCC panels, and presents the data observed. The Level 2 testing consisted of 54 impact tests in the NASA GRC Ballistic Impact Laboratory on 6- by 6-in. and 6- by 12-in. flat plates of RCC and evaluated two types of debris projectiles: BX-265 and PDL-1034 external tank foam. These impact tests helped determine the level of damage generated in the RCC flat plates by each projectile and validated the use of the foam and RCC models for use in LS-DYNA.

Melis, Matthew E.↗

DOE OSTI2020

Using the red chromatic coordinate to characterize the phenology of forest canopy photosynthesis

Vegetation phenology has received increasing attention in climate change research. Near-surface sensing using digital repeat photography has proven to be useful for ecosystem-scale monitoring of vegetation phenology. However, our understanding of the link between phenological metrics derived from digital repeat photography and the phenology of forest canopy photosynthesis is still incomplete, especially for evergreen plant species. Using 49 site-years of digital images from the PhenoCam Network from eight evergreen needleleaf forest (ENF) and six deciduous broadleaf forest (DBF) sites in North America, we explored the potential of the green chromatic (GCC) and red chromatic coordinates (RCC) in tracking forest canopy photosynthesis by comparing camera-derived start- and end-of-growing season (SOS and EOS, respectively) with corresponding estimates derived from eddy covariance-derived daily gross primary productivity (GPP). We found that for DBF sites, both GCC and RCC performed comparable in capturing SOS and EOS. However, similar to earlier studies, GCC had limited potential in capturing GPP-based SOS or EOS for ENF sites. In contrast, we found RCC was a better predictor of both GPP-based SOS and EOS for ENF sites. Environmental and ecological explanations were both provided that phenological transitions derived from RCC were highly correlated with spring and autumn meteorological conditions, as well as having overall higher correlations with phenology based on LAI, a critical variable for describing canopy development. Our results demonstrate that RCC is an underappreciated metric for tracking vegetation phenology, especially for ENF sites where GCC failed to provide reliable estimates for GPP-based SOS or EOS. Our results improve confidence in using digital repeat photography to characterize the phenology of canopy photosynthesis across forest types.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Rotating cylinder electrode in reactive CO 2 capture: Identifying active C species via transport, VLE models and kinetics

Here, this article explores technical challenges and potential methodologies for understanding electrochemical Reactive CO 2 Capture (RCC) mechanisms. RCC offers potential energy cost advantages by directly converting captured CO 2 into fuels and chemicals, unlike traditional carbon capture and utilization (CCU) processes that require sequential capture, concentration, and compression. However, direct conversion of captured CO 2 introduces complexity due to additional equilibrium buffer reactions, making it challenging to identify active species for reduction in electrochemical studies. This article discusses methods to integrate transport, thermodynamics, and kinetics concepts to identify active carbon sources in RCC. Vapor‐Liquid Equilibrium (VLE) and transport models are validated against experimental results obtained in a gastight rotating cylinder electrode reactor and are shown as useful tools for studying RCC in heterogeneous electrocatalysts across different capture agents, solvents, and temperatures. This article establishes an experimental framework for advancing research in electrochemical RCC.

Electrocatalysis↗

DOE OSTI2024

Corrosion and Enhanced Hydrogen Evolution in Electrochemical Reduction of Ammonium Carbamate on Transition Metal Surfaces

Experiments and theory are combined to search for catalyst activity and stability descriptors for the direct reactive capture and conversion (RCC) of CO 2 in ammonia capture solutions using Cu, Ag, Au, Sn, and Ti electrodes. Two major phenomena emerge in RCC that are not predominant in the electrochemical CO 2 reduction (CO 2 R) reaction, namely, the rapid corrosion and restructuring of the catalyst in the presence of the CO 2 -ammonia adducts and the promotion of the competing hydrogen evolution reaction (HER). The prevalence of HER in RCC is correlated to the electrostatic attraction of the protonated amine to the electrode and the repulsion of the captured CO 2 , using the potential of zero charge (PZC). The stability of catalysts under RCC conditions is a function of the applied potential and cannot be readily predicted using binding energy descriptors commonly used in the prediction of CO 2 R activity. Finally, a direct correlation between calculated binding energies of CO 2 R intermediates, atomic oxygen, hydrogen, and ammonia and the activity and stability of transition metals for RCC cannot be found, highlighting the need for descriptors beyond those known for CO 2 R.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2024

Enhancing risk and crisis communication with computational methods: A systematic literature review

Abstract Recent developments in risk and crisis communication (RCC) research combine social science theory and data science tools to construct effective risk messages efficiently. However, current systematic literature reviews (SLRs) on RCC primarily focus on computationally assessing message efficacy as opposed to message efficiency. We conduct an SLR to highlight any current computational methods that improve message construction efficacy and efficiency. We found that most RCC research focuses on using theoretical frameworks and computational methods to analyze or classify message elements that improve efficacy. For improving message efficiency, computational and manual methods are only used in message classification. Specifying the computational methods used in message construction is sparse. We recommend that future RCC research apply computational methods toward improving efficacy and efficiency in message construction. By improving message construction efficacy and efficiency, RCC messaging would quickly warn and better inform affected communities impacted by current hazards. Such messaging has the potential to save as many lives as possible.

Mathematical Methods In Social Sciences↗

DOE OSTI2025

Is the Chemisorbed CO 2 in Ionic Liquid Electrolytes Active for Electrochemical Utilization? A Case Study on Carboxylate and Carbamate Speciation

This study examines the activity of chemisorbed CO 2 species in the microenvironment formed by bifunctional ionic liquids (ILs) in the reactive capture and conversion (RCC) of CO 2 to CO on silver. Comparative electroanalytical measurements with imidazolium based ILs were performed to probe the impact of electrostatic interactions, anion and cation basicity, and hydrogen bonding on RCC. Particularly, ILs with 1-ethyl-3-methylimidazolium ([EMIM]+) and 1-ethyl-2,3-dimethylimidazolium ([EMMIM]+) cations and aprotic heterocyclic anions of 2-cyanopyrrolide ([2-CNpyr]) and 1,2,4-triazolide ([124-Triz]) were examined for RCC. It was found that anion–CO 2 carbamate complexes facilitate RCC at significantly lower overpotentials compared to cation–CO 2 carboxylate complexes. Additionally, [EMIM]+ was found to better stabilize anion–CO 2 complexes at the interface than [EMMIM]+. Furthermore, it was found that 2-CNpyrH that naturally forms during CO 2 absorption competes for electrode surface adsorption with the anion–CO 2 carbamate complex, thereby reducing the electrochemical activity of the anion–CO 2 complex. These results highlight the importance of IL structure in tuning the interfacial interactions and suggest that ILs with anion-dominated CO 2 chemisorption enhances CO 2 utilization in RCC applications.

Coskun, Oguz Kagan [Case Western Reserve Univ., Cl↗

DOE OSTI2026

Metallic Phase-Free Zn-Al Mixed Oxide Dual Function Materials Enable High Co Selectivity in Reactive Carbon Capture From Dilute Streams

Scaling conventional carbon capture and utilization methods can be limited by cost and permitting issues associated with transportation of captured CO2. Reactive carbon capture (RCC), in which a single solid-phase dual function material (DFM) is used to both capture CO2 from dilute streams (e.g., flue gas) and catalytically convert the bound species to products in a single unit operation, has the potential to reduce energy and capital costs by over 50% relative to separate capture and conversion. To incentivize adoption, high-value products such as methanol and CO should be targeted. Appealingly, CO can be produced at atmospheric pressure, thereby lowering overall H2 demand; however, high reaction temperatures (> 600 degrees C) and the use of oxidizable transition metals, such as Ni, are often necessary to drive the reverse water-gas shift (RWGS) during reactive desorption of the bound CO2. The sensitivity of these transition metals to oxygen undercuts their utility in point source RCC. To further derisk RCC, it is essential to develop metallic-phase free DFMs that are insensitive to residual oxygen in flue gas and can achieve selective reactive desorption to CO at moderate pressures (< 400 degrees C). To this end, we have developed K-modified Zn-Al mixed oxides (K/ZnAlOx) to convert captured CO2 to CO with > 97% selectivity and yields up to 53% of captured CO2 at 400 degrees C. Complementary in situ spectroscopy studies revealed the role of K-modification in improving RCC performance of unmodified ZnAlOx. The top performing DFM was also subjected to extended RCC cycling with oxygen co-fed with CO2 during the capture test to assess durability under simulated flue gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗