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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.

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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
NASA NTRS2013

Mars Sample Return Using Commercial Capabilities: ERV Trajectory and Capture Requirements

Mars Sample Return was presented as the highest priority planetary science mission of the next decade [1]. Lemke et al. [2] present a Mars Sample Return mission concept in which the sample is returned directly from the surface of Mars to an Earth orbit. The sample is recovered in Earth Orbit instead of being transferred between spacecraft in Mars Orbit. This paper provides the details of this sample recovery in Earth orbit and presents as such a sub-element of the overall Mars sample return concept given in [2]. We start from the assumption that a Mars Ascent Vehicle (MAV), initially landed on Mars using a modified SpaceX Dragon capsule, has successfully delivered the sample, already contained within an Earth Return Vehicle (ERV), to a parking orbit around Mars. From the parking orbit, the ERV imparts sufficient Delta-V to inject itself into an earthbound trajectory and to be captured into an Earth orbit eventually. We take into account launch window and Delta-V considerations as well as the additional constraint of increased safety margins imposed by planetary protection regulations. We focus on how to overcome two distinct challenges of the sample return that are driven by the issues of planetary protection: (1) the design of an ERV trajectory meeting all the requirements including the need to avoid contamination of Earth's atmosphere; (2) the concept of operations for retrieving the Martian samples in Earth orbit in a safe way. We present an approach to retrieve the samples through a rendezvous between the ERV and a second SpaceX Dragon capsule. The ERV executes a trajectory that brings it from low Mars orbit (LMO) to a Moon-trailing Earth orbit at high inclination with respect to the Earth-Moon plane. After a first burn at Trans-Earth Injection (TEI), the trajectory uses a second burn at perigee during an Earth flyby maneuver to capture the ERV in Earth orbit. The ERV then uses a non-propulsive Moon flyby to come to a near-circular Moon-trailing orbit. To perform the Earth Orbit Rendezvous (EOR), a second Dragon capsule is then launched from Earth and a similar lunar flyby is performed to rendezvous with the ERV. The requirements for rendezvous, close proximity operations and capture of the sample canister are described. A concept of operations for sample retrieval is presented along with design specifications of the ERV, the required modifications to the Dragon capsule, as well as the hardware, software, sensors, actuators, and capture mechanisms used. In our concept, a container is mounted to the front hatch of Dragon, capable of accommodating the sample canister and sealing it from the rest of the capsule. The sample canister is captured using a robotic arm with a magnetic grappling mechanism. Dragon then performs a propulsive maneuver to return to Earth for a controlled re-entry while the ERV (sans sample container) is left in the Moon trailing orbit. Contingency cases and related mitigation strategies are also discussed, including the advantages and disadvantages of performing the ERV rendezvous with a crew.

Faber, Nicolas F.↗
NASA NTRS2014

Asteroid Redirect Robotic Mission: Robotic Boulder Capture Option Overview

The National Aeronautics and Space Administration (NASA) is currently studying an option for the Asteroid Redirect Robotic Mission (ARRM) that would capture a multi-ton boulder (typically 2-4 meters in size) from the surface of a large (is approximately 100+ meter) Near-Earth Asteroid (NEA) and return it to cislunar space for subsequent human and robotic exploration. This alternative mission approach, designated the Robotic Boulder Capture Option (Option B), has been investigated to determine the mission feasibility and identify potential differences from the initial ARRM concept of capturing an entire small NEA (4-10 meters in size), which has been designated the Small Asteroid Capture Option (Option A). Compared to the initial ARRM concept, Option B allows for centimeter-level characterization over an entire large NEA, the certainty of target NEA composition type, the ability to select the boulder that is captured, numerous opportunities for mission enhancements to support science objectives, additional experience operating at a low-gravity planetary body including extended surface contact, and the ability to demonstrate future planetary defense strategies on a hazardous-size NEA. Option B can leverage precursor missions and existing Agency capabilities to help ensure mission success by targeting wellcharacterized asteroids and can accommodate uncertain programmatic schedules by tailoring the return mass.

Mazanek, Daniel D.↗
NASA NTRSDate not supplied

Atmospheric Mining in the Outer Solar System: Aerospacecraft Analysis, Propulsion, and Resource Capturing Implications

Atmospheric mining in the outer solar system has been investigated as a means of fuel production for high energy propulsion and power. Fusion fuels such as Helium 3 (3He) and deuterium can be wrested from the atmospheres of Uranus and Neptune and either returned to Earth or used in-situ for energy production. Helium 3 and deuterium were the primary gases of interest with hydrogen being the primary propellant for nuclear thermal solid core and gas core rocket-based atmospheric flight. A series of analyses were undertaken to investigate resource capturing aspects of atmospheric mining in the outer solar system. This included the gas capturing rate, storage options, and different methods of direct use of the captured gases. While capturing 3He, large amounts of hydrogen and 4He are produced. With these two additional gases, the potential for fueling small and large fleets of additional exploration and exploitation vehicles exists. Analyses of orbital transfer vehicles (OTVs), landers, and in-situ resource utilization (ISRU) mining factories are included. Preliminary observations are presented on near-optimal selections of moon base orbital locations, OTV power levels, and OTV and lander rendezvous points. Aerospacecraft with closed cycle gas core propulsion are used to capture the 3He and deuterium from the outer planet atmospheres. Additional analyses of aerospacecraft sizing led to important results, reducing the overall mining system mass by many thousands of metric tons. Earlier analyses had focused on small aerospacecraft payloads. Important influences on mining time in the atmosphere were also analyzed and will be presented.

In Situ Resource Utilization↗
NASA NTRSDate not supplied

Capturing, Analyzing, Maintaining, and Disseminating Shape Memory Material Data Between Information Management Systems

With an increased demand on reducing the time, cost, and effort to develop new materials, Integrated Computational Materials Engineering (ICME) has received widespread attention in various engineering disciplines as a catalyst for significantly reducing experimental testing during the material design process. An ICME approach to design can enable ‘fit-for-purpose’ materials to be realized in engineering applications by incorporating well-understood process-property-performance relationships between the various length and time scales in a material’s structure, enabling material optimization. However, such an approach requires validated multiscale models at the various length scales for a material, which in turn requires a large amount of data, a robust means of storing the data, and the ability to link data to developed material models. The NASA Vision 2040 [1] has identified nine key elements to enabling ICME approaches in system level design, with one being “Data, Information, and Visualization”, thus outlining the importance of a robust information management system for ICME. As the relationship between microstructure, properties, and material performance become better understood and incorporated into multiscale models that can be leveraged in application design, the emergence of new materials with application-driven properties can be realized. One such new material class that has seen growing attention are shape memory materials (SMM), in which a material can transition between a deformed and undeformed state via a reversible phase transformation when subject to a thermal, mechanical, or magnetic load [2]. SMMs have been used widely in aerospace and biomedical industries, including applications such as actuators, low-shock mechanisms, medical staples, braces, and stents [3, 4]. These materials exhibit unique behavior due to their ability to transition between phases, and thus the mechanisms that enable this transition must be captured in a data information management system and incorporated into SMM material models. At NASA Glenn Research Center, the Shape Memory Materials Database (SMMD) Tool has been developed to capture the necessary information that governs SMM material behavior and provide users the ability to select and visualize various SMMs for a specific application [5]. The database contains point-wise data for published SMM materials, along with the pedigree metadata for traceability necessary for a robust information management system. The database is also capable of storing in-house test data performed at NASA GRC by interacting with the developed Shape Memory Alloy (SMA) Analytics tool to extract the necessary point-wise values and populate the database. Although the SMMD Tool offers its users a single, authoritative source for SMM material data that is critical for model development and material design, the full material pedigree of the in-house test data for SMMs is not currently captured and is out of the scope for the SMMD tool. In this work, the schema for capturing SMM test data within the larger NASA GRC ICME Schema [6, 7, 8, 9] will be developed and implemented for thermomechanical tests conducted at NASA GRC. The developed schema will not only store the relevant data needed for the SMMD tool, but also the material pedigree (i.e., production of the bulk material, bulk material analysis, sample cut-out diagrams, sample fabrication procedure, etc.), test pedigree (i.e., test equipment used, measurement systems used, raw test data), and analysis pedigree (i.e., how the data in the SMMD tool is calculated). Furthermore, a Python-based framework will be developed to seamlessly interact between the SMA Analytics and SMMD tools, which will write the full dataset and associated metadata to the GRC Information Management System before passing the required point-wise data to the SMMD tool. Data informatics is a key element of the NASA Vision 2040, which requires not only that data is stored and maintained throughout the material lifecycle, but that the data is also accessible and reusable such that material development efforts can be minimized. Therefore, for an ICME design approach to be realized, a centralized information management system that drives the ICME process must be able to communicate with other databases. The work that will be presented in this presentation will therefore not only demonstrate the ability of NASA GRC’s information management system to capture SMM data, but also its ability to interact with pre-existing tools specialized for such materials.

Data management↗
DOE OSTI2020

Transition group metals for the capture of radioactive xenon

A xenon capture system that reduces the concentration of xenon in a carrier gas is disclosed. An example xenon capture system includes a carrier gas with a first concentration of xenon that flows through an intake into a chamber. Within the chamber is a reaction area that has at least one peripheral sidewall. The reaction area operates at a predetermined temperature, flow rate, and low pressure. Within the reaction area is at least one xenon capture mechanism that is at least partially formed of a transition metal. When the carrier gas is exposed to the xenon capture mechanism, the xenon capture mechanism adsorbs xenon from the carrier gas. The carrier gas, with a second concentration of xenon, exits the chamber through the exhaust outlet.

42 ENGINEERING↗
DOE OSTI2021

Turbomachine component with coating-capturing feature for thermal insulation

The disclosure relates to turbomachine components which include one or more coating-capturing features for thermal insulation. A turbomachine component may include: a body having an exterior surface positioned within a hot gas path (HGP) section of a turbomachine; and a coating-capturing feature mounted on the exterior surface of the body and in thermal communication with the HGP section of the turbomachine, wherein the coating-capturing feature comprises: a first member positioned on the exterior surface of the body, the first member having at least one outer sidewall defining a first perimeter of the coating-capturing feature, a second member positioned on the first member and having at least one outer sidewall defining a second perimeter of the coating-capturing feature, wherein the first member separates the second member from the exterior surface of the body, and an indentation positioned between the first and second members.

Berry, Jonathan Dwight↗
DOE OSTI2022

Techno-Economic Analysis and Optimization of Integrated NGCC-MEA System at High CO2 Capture Levels

This poster contains preliminary results for an ongoing analysis of modeling and optimization of an NGCC plant with a solvent-based CO2 capture system with high levels of CO2 capture – up to and beyond net-zero emissions. The work was performed to understand the incremental cost of high capture in order to compare with direct-air capture and other net-negative technologies, as well as to understand optimal operation and design of the CCS unit to achieve high capture with minimal increase in cost.

Deshpande, Anuja↗
DOE OSTI2024

Performance and Economic Evaluation of sCO2 Bottoming Cycles for Natural Gas Combined Cycle Plants with Capture

Natural gas combined cycles (NGCCs) with carbon capture are expected to play a significant role in decarbonization of the power generation sector. NGCC plants generally use triple pressure reheat steam Rankine power cycles for the bottoming cycle. Some studies in the literature have investigated the application of recompression and cascade style supercritical CO2 (sCO2) cycles for NGCC bottoming cycle applications but these studies have focused on power plants without carbon capture. However, NGCC plants fitted with post-combustion solvent-based CO2 capture systems will require a significant amount of steam for solvent regeneration and this can have a major impact on the optimal sCO2 bottoming cycle design. This study investigates the performance and economic potential of sCO2 bottoming cycles for H-class gas turbine based NGCC plants with a post-combustion capture system. A portion of the gas turbine exhaust heat is used for generation of steam required for solvent-based capture system while the rest of the waste heat is utilized in an sCO2 bottoming cycle for power generation. Overall, the performance and LCOE of investigated sCO2 bottoming cycles is similar to that of a state-of-the-art triple pressure reheat steam Rankine cycle. As the gas turbine exhaust temperature increases (beyond 630oC), sCO2 bottoming cycles begin to show greater performance and economic benefits compared to a steam Rankine cycle.

Pidaparti, Sandeep↗
DOE OSTI2023

Modeling Advanced Strippers for CO2 Capture from Gas-Fired Power Plants using Aqueous Piperazine

Energy performance of 5 m piperazine was evaluated with an advanced stripper at the pilot scale, accounting for heat loss. Modeling studies indicated that heat loss at locations other than the heat source impacted the heat duty. For strippers with excess packing, the column was the most important source of heat loss, and values as low as 0.03 GJ/hr can cause pinch and reabsorption of CO2. Solvents like 5 m PZ are more affected by heat loss in the column due to a top-side temperature pinch at high lean loading. Heat loss impacts NGCC CO2 capture more than coal-based CO2 capture. Surface temperature measurements pilot plants showed that heat loss was 50-75% controlled by natural convection. Measured heat loss was correlated with steam flowrate and wind speed and ranged from 8126 to 219668 Btu/hr, representing 35% of the measured heat rate on average. Net heat duty linearly varied with CO2 removal at low lean loading and was similar for coal and NGCC conditions at fixed removal. At 90% removal, net heat duty was about 2.5 GJ/t with 4 and 12% CO2 in the flue gas. 7 At NGCC conditions, strippers with finite packing can benefit from a flashing feed to the top of the column by using a hot bypass. A flashing feed was linked to a reduction in irreversibility of the stripper from temperature driving forces. It also reduces heat duty by up to 6% at fixed packing height and reduces packing requirement for a fixed steam heater size compared to a warm bypass. Lean loading and lean solvent rate were effective handles to maximize profitability of a fixed stripper design at low gas price. High ambient temperature operation can benefit from low pressure stripping to about 0.18 lean loading at 150 ℃ to maintain the cyclic capacity at reduced rich loading. At low gas price, the capture plant was able to maximize profitability even with a high heat duty of 2.7-3.1 GJ/t at a lean loading of 0.2-0.22 mol/mol. Heat recovery by partial water vapor condensation in a gas-liquid exchanger can be replaced by a direct contact condenser (DCC). The DCC improved gas cooling and reduced heat duty compared to the CO2 exchanger at 0.2 lean loading. The DCC when used with a 150 ℃/5.5 bar stripper can reduce the cost of capture compared to the base case by $3- 4/tonne at 15 ft of packing (optimum) but increases cost of capture by $6/tonne with a 120 ℃/2 bar stripper and 10 ft of packing (optimum). The DCC can work effectively with a solvent with a high heat of absorption and thermal stability.

Suresh Babu, Athreya↗
DOE OSTI2024

Neutron-induced capture-to-fission cross section ratio measured at LANSCE

Capture-to-fission cross section ratios are used as an alternative to absolute cross section measurements. This is due to the simplification on the calculations and the reduction of the uncertainties with respect to an absolute measurement of the cross section by eliminating experimental complications like self-absorption, beam/target overlap and non-uniformities. Different capture-to-fission reactions have been measured through the years at the Los Alamos Neutron Science Center (LANSCE) at Los Alamos National Laboratory (LANL) using the Detector for Advanced Neutron Capture Experiments (DANCE) combined with different fission detectors. Some of these are a Parallel Plate Avalanche Counter (PPAC) to detect fission fragments (FF), and the NEUtron detector array at DANCE (NEUANCE) to detect fission neutrons. As DANCE detects the γ-rays produced in capture and fission reactions, the fission instrument placed inside the DANCE cavity is used to tag the fission γ-rays for background identification and subtraction. Some examples of capture-to-fission ratio measurements performed with DANCE in the last years are the 233 U, 235 U and 239 Pu. The measurement technique, the different setups, and other potential applications of the instruments will be explained.

Nuclear Criticality Safety Program (NCSP)↗
DOE OSTI2025

Exploring Phosphonium‐Based Anion Exchange Polymers for Moisture Swing Direct Air Capture of Carbon Dioxide

This study explores the performance and stability of ammonium and phosphonium-based polymeric ionic liquids (PILs) with methyl and butyl substituents in moisture-swing direct air capture of CO 2 . The polymers are synthesized with chloride counterions, followed by ion exchange to the bicarbonate ion, and tests for CO 2 capture capacity and stability under cyclic wet–dry conditions. The phosphonium polymer with methyl substituents [PVBT-MeP] demonstrates the highest CO 2 capture capacity at ≈510 µmol g⁻¹, attributed to minimal steric hindrance and stronger ion pairing with bicarbonate. However, oxidative degradation is detected by 31 P NMR spectroscopy after the moisture swing experiment, with the appearance of a phosphine oxide peak at 61.28 ppm, which indicates phosphorus oxidation as the primary degradation pathway. In contrast, the ammonium polymer with butyl substituents [PVBT-BuN] exhibits the highest stability, showing no degradation over five moisture swing cycles. Additional stability experiments in 0.5 m KHCO 3 solutions reveal no degradation for any PIL, suggesting that oxidative degradation is driven by dynamic acid-base reactions during the moisture swing cycles in the air. Furthermore, these findings reveal the potential of phosphonium-based PILs for moisture-swing direct air capture, achieving high capacity while highlighting the need for optimized stability through counterion and structural design.

36 MATERIALS SCIENCE↗
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 OSTI2026

A comparative assessment of the economic viability of nuclear-integrated direct air capture systems

Direct air capture (DAC) systems require heat and electricity to operate, which can be supplied by nuclear power plants (NPPs). In this study, the performance and cost of various conceptual nuclear-DAC systems are assessed, and their performance is compared with several non-nuclear options. Three nuclear-DAC systems are considered: (1) a liquid solvent direct air capture (L-DAC) system with heat supplied from natural gas (NG) and electricity supplied by an NPP, (2) an electrified L-DAC system, fully powered by electricity from an NPP, and (3) a solid sorbent direct air capture (S-DAC) system utilizing both heat and electricity generated by an NPP. Two nuclear technologies are considered: a pressurized water reactor and a high-temperature gas-cooled reactor. Under the medium conservatism scenario, the levelized cost of direct air capture (LCOD) for these systems range from $\$$310/tCO 2 to $\$$525/tCO 2 with the L-DAC system having an NG heat supply at the lower end of the range, and the electrified L-DAC system and the S-DAC system at the higher end of the range. Coupling with nuclear energy led to a 21 % reduction in LCOD for the L-DAC system with NG heat supply and a 29 % reduction for the S-DAC system when compared to fully NG-powered options. When powering the DAC system with grid electricity, the LCOD is highly dependent on the assumed electricity price and carbon intensity. The nuclear option is the cheaper choice when the price of low-carbon grid electricity exceeds $\$$95/MWh and $\$$45/MWh for the L-DAC and S-DAC systems, respectively.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Insights into the Enhanced Oxidative Thermal Stability of Nanoparticle Organic Hybrid Materials Developed for Carbon Capture and Energy Storage

Due to the growing need for Direct Air Capture (DAC) and integrated carbon capture and conversion technologies, CO 2 capture materials that can withstand a wide range of environmental conditions, including fluctuating ambient temperatures and high concentrations of oxidizing agents (i.e., oxygen and moisture), are critically needed. Liquid-like Nanoparticle Organic Hybrid Materials (NOHMs) have been proposed as candidates for DAC and electrolyte additives enabling sustainable energy storage (i.e., integrated CO 2 capture and conversion and flow batteries). Liquid-like NOHMs functionalized with an ionic bond have been shown to display greatly enhanced oxidative thermal stability compared to the untethered polymer. However, these studies were limited in terms of reaction conditions and the detailed mechanisms of the oxidative thermal degradation were not reported. In this work, a kinetic thermal degradation analysis was performed on NOHM-I-HPE and the neat polymer, Jeffamine M2070 (HPE), in both non-oxidative and oxidative conditions. NOHM-I-HPE displayed similar thermal stability to the untethered polymer in a nitrogen environment, but interestingly, the thermal stability of the ionically tethered polymer was significantly enhanced in the presence of air. This observed enhancement of oxidative thermal stability is attributed to the orders of magnitude larger viscosity of the liquid-like NOHMs compared to untethered polymer and the bond stabilization of the ionically tethered polymer in the NOHMs canopy. Further, spectroscopic analyses of the liquid residue revealed that in the presence of oxygen, the degradation of HPE and NOHM-I-HPE occurs through the formation of trace amounts of carbonyls. This study illustrated that NOHMs can serve as functional materials for sustainable energy storage applications because of their excellent oxidative thermal stability.

25 ENERGY STORAGE↗
DOE OSTI2023

Big Data Analysis and Technical Review of Regeneration for Carbon Capture Processes

Carbon capture remains an integral technology to mitigate pollution from one of the most prevalent greenhouse gases. CO 2 desorption/absorbent regeneration for both solid- and liquid-based systems is widely recognized as an energy-intensive and costly process operation. Consequently, tremendous work was devoted towards developing new absorbents and regeneration processes to promote their economic feasibility for extensive implementation. In this review, we broadly and deeply review more than 10,000 papers and extract the hidden trends of carbon capture and absorbents regeneration in the past few decades, using a novel data-mining analysis technique. We comprehensively analyzed an array of recent absorbent regeneration methods utilized in post-combustion, pre-combustion, carbon capture from industrial point sources, and direct air carbon capture, with an emphasis on sorbent and solvent-based techniques. In conclusion, advanced regeneration methods in these techniques were illustrated and discussed, followed by recommendations for further research efforts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Net Present Value Optimization of a Natural Gas Combined Cycle Plant with CO 2 Capture using a Water-Lean Solvent Considering Transient Electricity Price for Multiple Regions

Global CO 2 emissions are increasing at about a 1.5% rate per year. Fossil fuel-based plants are one of the main contributors to this rise. In the power generation industry, fossil fuel plants are dominant, and many plants are under development. In this study, a natural gas combined cycle (NGCC) power plant with postcombustion capture using a leading water-lean solvent is considered. For optimal design and operating schedule, large-scale dynamic optimization is undertaken for net present value (NPV) optimization. The first principle dynamic model of NGCC is developed, including a model of the highly efficient H-class gas turbines. For computational tractability of the dynamic optimization problem, a reduced-order model is developed by using the Hankel singular value decomposition. A waterlean solvent, N-(2-ethoxyethyl)-3-morpholinopropan-1-amine, is used for carbon capture. A model of the capture system is developed in Aspen Plus, which is used to develop a reduced-order model by using ALAMO, a machine learning software. In addition, a reduced model of the CO 2 compression system with a dehydration unit is also considered. The integrated system is used for NPV optimization by using the Python-based PYOMO platform. The PCC process is analyzed for three configurations-conventional packed bed, rotating packed bed (RPB), and a combination of RPB and direct contact cooler. The NPV optimization is performed for 14 regional markets by considering year-long clustered and continuous locational marginal price data with a 1 h interval. Optimization results show that the PCC can achieve 90% CO 2 capture with a positive NPV for six regions. Sensitivity studies conducted by using the PCC configurations indicate that the process is economically feasible for 9 regions out of 14 regional electricity markets with NPV values in the range of 33−540 $MM.

cabon capture↗
DOE OSTI2025

Improving Conversion of Captured CO 2 on Mixed-Oxide Dual-Function Materials by Low-Concentration Metal Promotion

Reactive carbon capture (RCC) is a promising nascent approach to harness the untapped resource of waste CO 2 to produce fuels and platform chemicals. However, process economics relies on the design of dual-function materials (DFMs) that exhibit maximal conversion of captured CO 2 and high selectivity toward valuable carbon products (e.g., CO). Herein, we report the use of low-concentration (ca. 0.5 wt %) metal promotors (Pt and Au) to improve the conversion of captured CO 2 on a Zn-Al mixed-oxide DFM by >30%, while also more than doubling per-cycle CO yield due to enhanced retention of captured CO 2 and H 2 activation. In situ DRIFTS of bound CO 2 on the DFMs showed distinctions in surface carbonate formation for the Pt- and Au-modified materials that were correlated with product evolution during the reactive desorption step of RCC. Particularly, Pt afforded superior H 2 activation but formed irreversibly-bound bicarbonates, compromising overall productivity, while the Na/Au/ZA DFM predominantly adsorbed CO 2 on Na sites, resulting in polydentate carbonates that are retained until higher temperatures before conversion to CO. In conclusion, these results indicate that adding a low concentration of oxidation-resistant noble metals, especially Au, is an effective strategy for improving key performance metrics of Zn-Al mixed-oxide DFMs to further advance the development of scalable RCC technologies.

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