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DOE OSTI2024

Utilizing 3D Mechanical Earth Models for Calibration and Validation in a Large-Scale Carbon Capture and Storage Project in North Dakota

Conference paper presented at 17th International Conference on Greenhouse Gas Control Technologies (GHGT-17), Calgary, Alberta, Canada, October 20–24, 2024. Three-dimensional (3D) mechanical earth models (MEMs) are pivotal in assessing geological sites for carbon dioxide (CO 2 ) storage and mitigating potential risks associated with storage and injection. The Energy & Environmental Research Center is exploring innovative carbon storage monitoring techniques at a CO 2 storage site near Beulah, North Dakota. These methods aim to provide lower-impact, faster feedback for commercial carbon capture and storage (CCS) projects. The research includes monitoring CO 2 injection using various approaches: 1) an automated, integrated modular monitoring station; 2) time-lapse electromagnetic (EM) field surveys; 3) drone-based surveillance; 4) time-lapse seismic techniques; and 5) advanced wellbore monitoring.

02 PETROLEUM↗

DOE OSTI2024

Advanced CO 2 Capture Solvent Systems for Dynamic Power Generation: Quarterly Research Performance Progress Report, QR4 (Q4FY24)

We developed an integrated Computational Fluid Dynamics (CFD) model to simulate the multi-physics coupled cooling process of mixed gas by cold water within a Direct Contact Cooler (DCC) equipped with a rotating packing bed (RPB). The model captures the interactions between fluid dynamics, heat transfer, mass transport, and phase transitions, while accounting for key operational variables such as RPB rotational speed and the mass flow rates of both liquid and gas. The CFD model has been validated using experimental data, specifically by comparing predicted outflow gas and liquid temperatures to measured results. Our findings demonstrate the significant effects of RPB rotational speed and mass flow rates on cooling performance, providing valuable insights for optimizing DCC efficiency in industrial applications.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2023

Analysis of Carbon Capture Retrofits for Cement Plants

The objective of this study is to provide an estimate of the cost to capture CO 2 in retrofit applications at cement plants. The cement plant configurations considered in this study include natural gas and solid fuel (coal and coke) cases, and both wet- and dry kiln-fed plant designs, however the base cement plants in this study were not evaluated other than characterization of their kiln off-gas stream and high-level quantification of heat integration potential at the existing plant. In each case, the base cement plant produces 1.5 M tonnes per year of finished cement, assuming 91.4 percent clinker content. This analysis includes a 10 percent retrofit cost increase for process integration and low grade heat recovery, when compared to the analogous non-heat integration case. Heat integration is considered as a potential offset to capture system heating demands (i.e., as a percentage reduction). Recovery and reuse of excess heat from the base cement plant can provide economic benefits—primarily by reducing the need to purchase supplemental natural gas for CO 2 solvent regeneration—but any process improvement must be great enough to overcome the cost increases (i.e., capital and O&M) necessary to realize those benefits. With heat integration potential of 10 percent and 30 percent, that benefit wasn’t significant enough to offset the increase in capital and operating costs, and a cost of capture increase was observed based on the assumptions in this report. Benefits of heat integration potential may be realized when natural gas prices are higher, as demonstrated in the sensitivity to natural gas price where crossover points exist between heat integration cases and their respective non-heat integration cases. Four of the base cases were further evaluated to explore the cost implications of deeper levels of gas pre-treatment to remove oxides of nitrogen (NOx) and oxides of sulfur (SOx) from the kiln off-gas stream prior to CO 2 capture, purification, and compression. The results of these additional case analyses showed a 7.4–18.8 percent increase in cost of capture over the respective base case (i.e., analogous cases without SOx/NOx removal).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

The Influence of Disk Composition on the Evolution of Stars in the Disks of Active Galactic Nuclei

Abstract Disks of gas accreting onto supermassive black holes, powering active galactic nuclei (AGN), can capture stars from nuclear star clusters or form stars in situ via gravitational instability. The density and thermal conditions of these disks can result in rapid accretion onto embedded stars, dramatically altering their evolution in comparison to stars in the interstellar medium. Theoretical models predict that, when subjected to sufficiently rapid accretion, fresh gas replenishes hydrogen in the cores of these stars as quickly as it is burned into helium, reaching a quasi-steady state. Such massive, long-lived (“immortal”) stars may be capable of dramatically enriching AGN disks with helium, and would increase the helium abundance in AGN broad-line regions relative to that in the corresponding narrow-line regions and hosts. We investigate how the helium abundance of AGN disks alters the evolution of stars embedded therein. We find, in agreement with analytical arguments, that stars at a given mass are more luminous at higher helium mass fractions, and so undergo more radiation-driven mass loss. We further find that embedded stars tend to be less massive in disks with higher helium mass fractions, and that immortal stars are less common in such disks. Thus, disk composition can alter the rates of electromagnetic and gravitational wave transients as well as further chemical enrichment by embedded stars.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Integrated Ammonia Capture and Exchange on Ion‐Exchanged 4A Zeolites

Ammonia poses a challenge in effluent gas streams due to its corrosive nature. However, in fusion settings tritiated ammonia can be formed, leading to both tritium loss in inventory and the generation of reactive species. Therefore, identifying pathways in which both tritium can be recovered, and the ammonia can be easily handled would be beneficial. One such way to do so would be to combine two useful techniques: ammonia sequestration and hydrogen exchange (ND 3 →NH 3 ). However, materials that can both adsorb ammonia and subsequently perform reactions on ammonia have not been well explored. Here, in this work, we present the development of ion-exchanged A-type zeolites to be utilized as a support material for platinum catalysts. In this way, the zeolite can adsorb ammonia and the platinum catalyst can facilitate hydrogen exchange allowing for bifunctional reactivity of the material to be achieved. A variety of elements were explored for their effect on A-type zeolites and resulted in an isotopic difference in the adsorption of ND 3 and NH 3 , noting the use of deuterium as a surrogate for tritium. Several platinum-impregnated zeolites were able to remove ND 3 from the gas stream, indicating that utilizing these materials in isotope recovery processes would improve accountability of these valuable hydrogen isotopes.

Koch, Christopher J. [Savannah River National Labo↗

NASA NTRS1987

Nucleogenic noble gas components in the Cape York iron meteorite

The paper reports data on neutron capture products of the secondary cosmic ray component, the inferred proton and neutron fluences, and the identification of double beta decay of Se-82 in heavily shielded samples of the Cape York iron meteorite. One purpose of this study is to develop a new chronometer for cosmic ray exposure, based on the nuclides I-129 (16 My half-life) and Xe-129 from low energy cosmic ray reactions on Te. The abundance ratio of these two nuclides permits the determination of an (effective) exposure age of 93 + or - 16 My, which represents the first exposure age datum of Cape York. The very small concentrations of spallogenic Ar-38 = 6.5 x 10 to the -10th cu cm STP/g in the metal and troilite (per g Fe) document the heavily shielded locations of the sample. An excess of Xe-129 in the troilite is shown to be entirely due to the decay of cosmic-ray-produced I-129. On the other hand, an inclusion in the troilite reveals the presence of Xe-129 from extinct I-129 and documents its about 4.5 Gy formation age. Mono-isotopic excess of Kr-82 is identified as due to beta-beta-decay of Se-82 with an inferred half-life of 1.0 x 10 to the 20th y. This represents the first beta-beta-decay product observed in a meteorite.

Murty, S. V. S.↗

NASA NTRS1991

Aerodynamic design of gas and aerosol samplers for aircraft

The aerodynamic design of airborne probes for the capture of air and aerosols is discussed. Emphasis is placed on the key parameters that affect proper sampling, such as inlet-lip design, internal duct components for low pressure drop, and exhaust geometry. Inlet designs that avoid sonic flow conditions on the lip and flow separation in the duct are shown. Cross-stream velocities of aerosols are expressed in terms of droplet density and diameter. Flow curvature, which can cause aerosols to cross streamlines and impact on probe walls, can be minimized by means of a proper inlet shape and proper probe orientation, and by avoiding bends upstream of the test section. A NASA panel code called PMARC was used successfully to compute streamlines around aircraft and probes, as well as to compute to local velocity and pressure distributions in inlets. A NACA 1-series inlet with modified lip radius was used for the airborne capture of stratospheric chlorine monoxide at high altitude and high flight speed. The device has a two-stage inlet that decelerates the inflow with little disturbance to the flow through the test section. Diffuser design, exhaust hood design, valve loss, and corner vane geometry are discussed.

Soderman, Paul T.↗

DOE OSTI2022

Diamine solvent system for CO 2 capture

Disclosed herein is a method and system for CO 2 removal from a gas stream using a diamine solvent having a Formula I R 1 (R 2 )N-L 1 -NH-R 3 . With respect to Formula I, each of R 1 and R 2 independently is aliphatic, cycloaliphatic, or R 1 and R 2 together with the nitrogen to which they are attached, form a heterocyclyl ring; L 1 is aliphatic, cycloaliphatic, or L 1 and R 1 together with the nitrogen to which they are attached form a heterocyclyl ring; and R 3 is aliphatic, cycloaliphatic, cycloalkylalkyl, or alkoxyalkyl. And/or the compound may have a viscosity of less than 75 cP at a CO 2 -loading of 40 mol % and at a temperature of 40° C.

Malhotra, Deepika↗

DOE OSTI2023

Diamine solvent system for CO 2 capture

Disclosed herein is a method and system for CO 2 removal from a gas stream using a diamine solvent having a Formula I R 1 (R 2 )N-L 1 -NH—R 3 Formula I. With respect to Formula I, each of R 1 and R 2 independently is aliphatic, cycloaliphatic, or R 1 and R 2 together with the nitrogen to which they are attached, form a heterocyclyl ring; L 1 is aliphatic, cycloaliphatic, or L 1 and R 1 together with the nitrogen to which they are attached form a heterocyclyl ring; and R 3 is aliphatic, cycloaliphatic, cycloalkylalkyl, or alkoxyalkyl. And/or the compound may have a viscosity of less than 75 cP at a CO 2 -loading of 40 mol % and at a temperature of 40° C.

Malhotra, Deepika↗

DOE OSTI2022

A scalable solid-state nanoporous network with atomic-level interaction design for carbon dioxide capture

Carbon capture and sequestration reduces carbon dioxide emissions and is critical in accomplishing carbon neutrality targets. Here, we demonstrate new sustainable, solid-state, polyamine-appended, cyanuric acid–stabilized melamine nanoporous networks (MNNs) via dynamic combinatorial chemistry (DCC) at the kilogram scale toward effective and high-capacity carbon dioxide capture. Polyamine-appended MNNs reaction mechanisms with carbon dioxide were elucidated with double-level DCC where two-dimensional heteronuclear chemical shift correlation nuclear magnetic resonance spectroscopy was performed to demonstrate the interatomic interactions. We distinguished ammonium carbamate pairs and a mix of ammonium carbamate and carbamic acid during carbon dioxide chemisorption. The coordination of polyamine and cyanuric acid modification endows MNNs with high adsorption capacity (1.82 millimoles per gram at 1 bar), fast adsorption time (less than 1 minute), low price, and extraordinary stability to cycling by flue gas. This work creates a general industrialization method toward carbon dioxide capture via DCC atomic-level design strategies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Sorption Enhanced Mixed Matrix Membranes for Hydrogen (H 2 ) Purification and Carbon Dioxide (CO 2 ) Capture

The technical objective of this project was to develop sorption enhanced mixed matrix membranes with H 2 permeance of 500 gas permeance units (GPU) and H 2 /CO 2 selectivity of 30 at 150-200 °C. These membranes will be the central component in the design of membrane based systems for 90% capture of CO 2 from coal-derived syngas, with 95% CO 2 purity at a cost of electricity 30% less than baseline capture approaches. The unique approach in this proposal is to design crosslinked polymers containing Pd-based nanoparticles achieving strong H 2 sorption and size sieving ability and thus H 2 /CO 2 selectivity. The specific objectives for each budget period (BP) are described below. BP 1: Identify polymer matrix with strong size sieving ability and palladium (Pd)-containing nanomaterials to prepare freestanding mixed matrix films with H 2 permeability of 50 Barrer and H 2 /CO 2 selectivity of 30 at 150-200°C with simulated syngas. BP 2: Prepare and optimize thin film mixed matrix composite membranes materials with H 2 permeance of 500 GPU and H 2 /CO 2 selectivity of 30 at 150-200 °C, and complete the modification of the membrane test unit for the field test in the BP 3. BP 3: Conduct a 20-day field test of the membranes with real syngas at Center for Advanced Energy Research (CAER) of the University of Kentucky (UKy). During the BP2, we have successfully prepared thin-film composite (TFC) membranes based on mixed matrix materials (MMMs) containing Pd nanoparticles in polymers, and demonstrated their superior and robust performance for H 2 /CO 2 separation at 150 – 225 °C. (1) Production of the Pd based nanoparticles with a diameter of 4 nm has been scaled up to 200 mg/day. (2) We have prepared TFC membranes with H 2 permeance above 500 GPU and H 2 /CO 2 selectivity above 30 at temperatures up to 225 °C, which meet the targets for the BP2. (3) We have conducted parametric studies of TFC membranes with a mixed gas containing H 2 S and H 2 O and demonstrated the stability of the membranes. (4) We have established a new testing plan at the Center for Advanced Energy Studies (CAER) at the University of Kentucky because NCCC decided to shut down their gasifier. During this project, four Ph.D. students received the inter-disciplinary training and graduated, including Shailesh Konda, Maryam Omidvar, Deqiang Yin, and Lingxiang Zhu. One postdoctoral researcher (Dr. Liang Huang) and two Ph.D. students (Abhishek Kumar and Hien Nguyen) are involved in this project. The project leads to one provisional patent application, eight peer-reviewed articles, and one manuscript in preparation. The details are shown below.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2022

Autoignition Delay Time Measurements and Chemical Kinetic Modeling of Hydrogen/Ammonia/Natural Gas Mixtures

Abstract In recent years, hydrogen-carrying compounds have accrued interest as an alternative to traditional fossil fuels due to their function as zero-emission fuels. As such, there is interest in investigating hydrogen-carrying compounds to improve understanding of the fuels’ characteristics for use in high-pressure systems. In the current study, the oxidation of ammonia/natural gas/hydrogen mixtures was carried out to study CO formation profiles as well as the ignition delay times behind reflected shock waves in order to refine chemical kinetic models. Experiments were carried out in the University of Central Florida’s shock tube facility by utilizing chemiluminescence to obtain OH* emission and laser absorption spectroscopy to obtain CO profiles. Experimental results were then compared with the GRI 3.0 mechanism, as well as the proprietary UCF 2022 mechanism utilizing CHEMKIN-Pro software. In general, both models were able to capture the trend in autoignition delay times and CO time histories for natural gas and ammonia mixtures. However, for ammonia-hydrogen mixtures, GRI 3.0 failed to predict ignition delay times whereas the UCF 2022 mechanism was able to capture the IDTs within the uncertainty limits of the experiments. A sensitivity analysis was conducted for different mixtures to understand the important reactions at the experimental conditions. Finally, a reaction pathway analysis was carried out to understand important ammonia decomposition pathways in the presence of hydrogen and natural gas.

Baker, Jessica B.↗

DOE OSTI2024

Direct air capture with amino acid solvent: Operational optimization using a crossflow air‐liquid contactor

Direct air capture (DAC) is a negative emission technology for removing CO2 from the atmosphere to maintain the CO 2 level within a reasonable range so as to address greenhouse effects. In this study, the operational optimization of lab-scale DAC has been investigated using a crossflow air-liquid contactor loaded with a three dimensionally printed Gyroid packing structure and a potassium sarcosinate solvent. The effects of various parameters, including feed air flow rate, liquid solvent flow rate, contactor geometry, and ambient temperature, are examined. The results demonstrate that the Gyroid packing design achieves comparable CO 2 capture performance to conventional packed beds but with a significantly lower pressure drop of up to 77.8%, suggesting its potential as an efficient and cost-effective solution for gas–liquid contactors in DAC. Additionally, the study explores the climate impact on CO 2 capture performance and finds that as the air temperature increases from 35 to 95°F at a fixed relative humidity of 80%, the CO 2 capture rate increased from 23.2% to 46.8% with better stability. The research highlights the importance of optimizing contactor design and operational conditions to improve the CO 2 capture rate and feasibility of DAC systems as a negative emission technology for addressing greenhouse effects.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1994

Small Particles Intact Capture Experiment (SPICE)

The Small Particles Intact Capture Experiment (SPICE) will develop technologies and engineering techniques necessary to capture nearly intact, uncontaminated cosmic and interplanetary dust particles (IDP's). Successful capture of such particles will benefit the exobiology and planetary science communities by providing particulate samples that may have survived unaltered since the formation of the solar system. Characterization of these particles may contribute fundamental data to our knowledge of how these particles could have formed into our planet Earth and, perhaps, contributed to the beginnings of life. The term 'uncontaminated' means that captured cosmic and IDP particles are free of organic contamination from the capture process and the term 'nearly intact capture' means that their chemical and elemental components are not materially altered during capture. The key to capturing cosmic and IDP particles that are organic-contamination free and nearly intact is the capture medium. Initial screening of capture media included organic foams, multiple thin foil layers, and aerogel (a silica gel); but, with the exception of aerogel, the requirements of no contamination or nearly intact capture were not met. To ensure no contamination of particles in the capture process, high-purity aerogel was chosen. High-purity aerogel results in high clarity (visual clearness), a useful quality in detection and recovery of embedded captured particles from the aerogel. P. Tsou at the Jet Propulsion Laboratory (JPL) originally described the use of aerogel for this purpose and reported laboratory test results. He has flown aerogel as a 'GAS-can Lid' payload on STS-47 and is evaluating the results. The Timeband Capture Cell Experiment (TICCE), a Eureca 1 experiment, is also flying aerogel and is scheduled for recovery in late April.

Nishioka, Ken-Ji↗

NASA NTRS2019

Evaluation of Ionic Liquids for Closed Air Revitalization

This document is the final report resulting from the work conducted by undergraduate students at the University of South Alabama during the 2018/2019 academic year and was prepared by the undergraduate students. As NASA pushes the boundaries further into space, the current technologies within the various life support systems must be improved upon. One such improvement is needed to the current air revitalization systems, specifically sorbents that can capture CO2 more effectively from enclosed habitats. Ionic liquids (ILs) have been considered as absorbents for flue gas, but little research has been done to test the ability of ILs at ambient pressures and relatively low concentration of CO2. The experiment outlined below utilizes the task-specific ionic liquid, tetramethylammonium taurinate (TMN), in a commercial off the shelf absorption system to capture CO2. The CO2 stream is combined with nitrogen to produce an inlet gas concentration relevant to close air revitalization applications. At an inlet gas flow with a CO2 partial pressure of 3.8 torr the system was capable of removing just under 97% of the inlet CO2. The concentration of CO2 in the outlet stream, partial pressure 0.16 torr, was less than that of atmospheric air. The duty required to separate the absorbed gas from the ionic liquid as well to cool the ionic liquid to be reintroduced to the column were acquired utilizing laboratory cooling/heating baths. These results show that TMN may be an efficient candidate for consideration in closed air revitalization.

Duck, Gerald↗

DOE OSTI2021

Amino‐Functionalised Hybrid Ultramicroporous Materials that Enable Single‐Step Ethylene Purification from a Ternary Mixture

Abstract Pyrazine‐linked hybrid ultramicroporous (pore size <7 Å) materials (HUMs) offer benchmark performance for trace carbon capture thanks to strong selectivity for CO 2 over small gas molecules, including light hydrocarbons. That the prototypal pyrazine‐linked HUMs are amenable to crystal engineering has enabled second generation HUMs to supersede the performance of the parent HUM, SIFSIX‐3‐Zn , mainly through substitution of the metal and/or the inorganic pillar. Herein, we report that two isostructural aminopyrazine‐linked HUMs, MFSIX‐17‐Ni (17=aminopyrazine; M=Si, Ti), which we had anticipated would offer even stronger affinity for CO 2 than their pyrazine analogs, unexpectedly exhibit reduced CO 2 affinity but enhanced C 2 H 2 affinity. MFSIX‐17‐Ni are consequently the first physisorbents that enable single‐step production of polymer‐grade ethylene (>99.95 % for SIFSIX‐17‐Ni ) from a ternary equimolar mixture of ethylene, acetylene and CO 2 thanks to coadsorption of the latter two gases. We attribute this performance to the very different binding sites in MFSIX‐17‐Ni versus SIFSIX‐3‐Zn .

Mukherjee, Soumya↗

DOE OSTI2021

Amino‐Functionalised Hybrid Ultramicroporous Materials that Enable Single‐Step Ethylene Purification from a Ternary Mixture

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Mechanism of the Non‐Kasha Fluorescence in Pyrene

The high-energy shoulder in the gas-phase fluorescence emission spectrum of pyrene is a well-known example of non-Kasha emission. Here, we comparatively assess two approaches, vibronic perturbation theory and nonadiabatic dynamics, in their ability to predict and explain the gas-phase fluorescence spectrum of pyrene. While both methods qualitatively capture the non-Kasha emission, they differ in their computational requirements, accuracy, and physical interpretation. Vibronic perturbation theory and nonadiabatic dynamics are complementary and can be combined in a two-step approach to non-Kasha fluorescence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗