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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Carbon Dioxide Capture at Nucleophilic Hydroxide Sites in Oxidation‐Resistant Cyclodextrin‐Based Metal–Organic Frameworks**

Abstract Carbon capture and sequestration (CCS) from industrial point sources and direct air capture are necessary to combat global climate change. A particular challenge faced by amine‐based sorbents—the current leading technology—is poor stability towards O 2 . Here, we demonstrate that CO 2 chemisorption in γ‐cylodextrin‐based metal–organic frameworks (CD‐MOFs) occurs via HCO 3 − formation at nucleophilic OH − sites within the framework pores, rather than via previously proposed pathways. The new framework KHCO 3 CD‐MOF possesses rapid and high‐capacity CO 2 uptake, good thermal, oxidative, and cycling stabilities, and selective CO 2 capture under mixed gas conditions. Because of its low cost and performance under realistic conditions, KHCO 3 CD‐MOF is a promising new platform for CCS. More broadly, our work demonstrates that the encapsulation of reactive OH − sites within a porous framework represents a potentially general strategy for the design of oxidation‐resistant adsorbents for CO 2 capture.

Zick, Mary E.↗
DOE OSTI2022

Carbon Dioxide Capture at Nucleophilic Hydroxide Sites in Oxidation–Resistant Cyclodextrin–Based Metal–Organic Frameworks

Carbon capture and sequestration (CCS) from industrial point sources and direct air capture are necessary to combat global climate change. A particular challenge faced by amine-based sorbents—the current leading technology—is poor stability towards O 2 . Here, we demonstrate that CO 2 chemisorption in γ-cylodextrin-based metal-organic frameworks (CD-MOFs) occurs via HCO 3 – formation at nucleophilic OH – sites within the framework pores, rather than via previously proposed pathways. Here, the new framework KHCO 3 CD-MOF possesses rapid and high-capacity CO 2 uptake, good thermal, oxidative, and cycling stabilities, and selective CO 2 capture under mixed gas conditions. Because of its low cost and performance under realistic conditions, KHCO 3 CD-MOF is a promising new platform for CCS. More broadly, our work demonstrates that the encapsulation of reactive OH – sites within a porous framework represents a potentially general strategy for the design of oxidation-resistant adsorbents for CO 2 capture.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

High-Performance CO 2 Capture from Air by Harnessing the Power of CaO- and Superbase-Ionic-Liquid-Engineered Sorbents

Direct air capture (DAC) of CO 2 by solid porous materials represents an attractive “negative emission” technology. However, state-of-the-art sorbents based on supported amines still suffer from unsolved high energy consumption and stability issues. For this work, taking clues from the CO 2 interaction with superbase-derived ionic liquids (SILs), high-performance and tunable sorbents in DAC of CO 2 was developed by harnessing the power of CaO- and SIL-engineered sorbents. Deploying mesoporous silica as the substrate, a thin CaO layer was first introduced to consume the surface-OH groups, and then active sites with different basicities (e. g., triazolate and imidazolate) were introduced as a uniformly distributed thin layer. The as-obtained sorbents displayed high CO 2 uptake capacity via volumetric (at 0.4 mbar) and breakthrough test (400 ppm CO 2 source), rapid interaction kinetics, facile CO 2 releasing, and stable sorption/desorption cycles. Operando diffuse reflectance infrared Fourier transformation spectroscopy (DRIFTS) analysis under simulated air atmosphere and solid-state NMR under 13 CO 2 atmosphere demonstrated the critical roles of the SIL species in low-concentration CO 2 capture. The fundamental insights obtained in this work provide guidance on the development of high-performance sorbents in DAC of CO 2 by leveraging the combined advantages of porous solid scaffolds and the unique features of CO 2 -philic ionic liquids.

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

Systems Analysis of Biomass and Coal Co-firing Power Plants with Deep Carbon Capture Toward Net-zero Emissions

Achieving a net-zero emission economy in the United States requires integrating diverse low-carbon and negative-emission technologies into the existing fossil fuel-dominant power fleet. Potential technologies from the low-carbon portfolio include renewable power, fossil power with carbon capture and storage (CCS), bioenergy with CCS (BECCS), and direct air capture (DAC). Renewable power is a clean energy source but has to pair with costly battery storage to provide dispatchable electricity. Fossil power with CCS offers dispatchable electricity yet still relies on DAC to offset residual emissions, even when deploying deep CCS with more than 90% CO2 capture. Coal-biomass co-firing with CCS, a subset of BECCS, is a reliable energy production technology that can be retrofitted from existing electricity generation units (EGUs). Power plant retrofit maximizes the use of the current U.S. coal power fleet without the need for large-scale deployment of new renewable power, battery storage, or DAC. Retrofitting coal-biomass co-firing with deep CCS in EGUs is a promising option, but not a universal solution. Biomass co-firing at a power plant introduces economic challenges and indirectly poses pressure on land and water resources. Meanwhile, retrofitting deep CCS affects plant efficiency and raises electricity generation costs. Overall, the technical feasibility and economic viability of plant retrofits vary across EGUs, as they are contingent upon the regional availability of biomass, unit-specific characteristics, site-specific fuel supply costs, and adjacent CO2 storage potential. Government incentives like 45Q can improve the retrofit viability, though the impact requires further quantification. A comprehensive analysis at the unit level is essential to address the question regarding the fate of the U.S. coal-fired electricity generation fleet toward the net-zero emission goal. This study conducts a systematic techno-economic-environmental assessment of EGUs to identify the viability of biomass co-firing and deep CCS retrofits in the U.S. coal-fired power fleet. Specifically, it characterizes the techno-economic performance of deep carbon capture, estimates life cycle greenhouse gas (GHG) emissions, and conducts a fleet-level assessment on retrofit viability. The key objectives are (1) to estimate the unit-specific performance and retrofitted cost under various biomass co-firing levels and CO2 capture rates; (2) to determine the possibility of reaching net-zero emission at the fleet level; (3) to quantify the cumulative capacities that are suitable for plant retrofits under current and future biomass supply scenarios; and (4) to improve the understanding of policy impacts on such retrofits to help the power sector’s transition to a net-zero economy. Techno-economic Model of Deep Carbon Capture. This study develops the performance and economic models for Monoethanolamine-based post-combustion CO2 capture at 95–99% capture rates. The process is simulated in Aspen Plus, analyzing the performance of carbon capture technology by varying the plant sizes, solvent lean loading, CO2 concentrations, and flue gas inlet temperature. Based on the key inputs and output parameters of CO2 capture, a reduced-order performance model of deep carbon capture is formulated. In addition, an engineering-economic model integrating the performance metrics is developed to estimate the capital as well as operation and maintenance (O&M) costs. Capital cost estimations follow the framework of the Integrated Environmental Control Model (IECM) and incorporate data regressions from three technical reports by IECM, the National Energy Technology Laboratory (NETL), and the National Renewable Energy Laboratory. The O&M cost estimation utilizes the actual inventory consumption rate and labor requirements. Both performance and cost models are embedded into IECM v13.0-beta, a fossil-fuel power plant modeling tool. Life Cycle Assessment of Power Plants. This study estimates the GHG emissions of power plants through life cycle assessment (LCA). The LCA scope includes fuel supply, combustion-based power generation, and CO2 transport and storage. The fuel-based life cycle module is designed following the framework of the NETL Unit Process Library and CO2U LCA Guidance Toolkit. The module is then incorporated into IECM v13.0-beta. The process-based LCA is applied to estimate the GHG emissions of coal and biomass supply, coal- and coal-biomass co-firing power plant operation, as well as CO2 pipeline transport and geographical sequestration. An uncertainty analysis is conducted to quantify the variability and uncertainty associated with the LCA using the Latin Hypercube Sampling (LHS) method. Fleet-level Assessment. This study evaluates the technical and economic feasibility of selected coal-fired EGUs, examines the role of tax credits in retrofit viability, and assesses the competitiveness of retrofitted units against other low-carbon options. Unit screening identifies EGUs for the study, focusing on new, efficient baseload units with air pollution controls. The power plant databases are then established to organize unit-specific information on performance and operating conditions from the relevant public databases. Biomass for co-firing retrofits is selected based on home and neighboring county availability, ensuring sustained operation with at least a 5% co-firing level. The CO2 storage site is determined by state-level storage potential, with ArcGIS Pro and NETL CO2 Saline Storage Cost Model used to identify the optimal balance between the nearest transport distances and affordable storage costs. The latest IECM v13.0-beta is then employed to configure and evaluate the eligible EGUs with or without the deployment of deep CCS and biomass co-firing. A supply curve is established to illustrate the cumulative installed capacity suitable for retrofits at different cost levels. A sensitivity analysis on tax credits for carbon sequestration is performed. Finally, a unit-level cost comparison is conducted among retrofitted plants, renewable power with battery storage, and abated fossil fuels with DAC. Expected Results. This study evaluates the technical, economic, and environmental metrics of each EGU across an array of CO2 capture rates and biomass co-firing level scenarios. Unit-level comparisons will identify critical factors influencing technical performance. The supply curves with and without tax incentives will provide insights into the impact of tax credits on biomass co-firing and CCS deployment. The cost comparisons with renewables and DAC-retrofit will assess the competitiveness of the retrofitted units. Life cycle emissions from each unit will be assessed to identify the scenarios under which net-zero emissions can be achieved. These analyses are expected to determine the total coal-fired capacity suitable for serving as a low-carbon energy source with or without tax incentives. The study results are novel in identifying optimal unit-specific strategies for producing carbon-neutral power, whether through retrofitting EGUs with deep CCS, biomass co-firing, DAC, or installing renewable power with battery. The findings will provide insight into nationwide efforts to ensure reliable, affordable, and low-carbon electricity. It also will inform investment decisions and policies in the deployment of deep carbon capture and negative emission technologies for a net-zero energy future.

Biomass Co-firing↗
DOE OSTI2022

The status and prospects of materials for carbon capture technologies

In order to combat climate change, carbon dioxide (CO 2 ) emissions from industry, transportation, buildings, and other sources need to be captured and long-term stored. Decarbonization of these sources requires special types of materials that have high affinities for CO 2 . Potassium hydroxide is a benchmark aqueous sorbent that reacts with CO 2 to convert it into K 2 CO 3 and subsequently precipitated as CaCO 3 . Another class of carbon capture materials is solid sorbents that are usually functionalized with amines or have natural affinities for CO 2 . The next wave of materials for carbon capture under investigation includes activated carbon, metal–organic frameworks, zeolites, carbon nanotubes, and ionic liquids. In this issue of MRS Bulletin, some of these materials are highlighted, including solvents and sorbents, membranes, ionic liquids, and hydrides. Other materials that can capture CO2 from low concentrations of gas streams, such as air (direct air capture) are also discussed. Also covered in this issue are machine learning-based computer algorithms developed with the goal to speed up the progress of carbon capture materials development, and to design advanced materials with high CO 2 capacity, improved capture and release kinetics, and improved cyclic durability.

36 MATERIALS SCIENCE↗
DOE OSTI2021

FEED Study of Carbon Capture Inc. DAC and CarbonCure Utilization Using United States Steel's Gary Works Waste Plant

Direct Air Capture (DAC) has been proposed as a means of reducing atmospheric concentrations of CO2. While DAC has been evaluated through lab-scale, bench-scale, and small-scale pilot units, large-scale deployment has not been achieved. Feasibility studies are one tool to understand the potential design, operation, performance, and impact of commercial-scale DAC. This paper presents the results of a feasibility study for a passive DAC system deployed at >100,000 tpy scale in three different regions across the U.S. and awarded to Carbon Collect by the U.S. Department of Energy National Energy Technology Laboratory (DOE NETL). The MechanicalTree™technology has been designed and engineered by Carbon Collect based on the concept initially developed at Arizona State University Center for Negative Carbon Emissions. It uses a tower of stacked, sorbentcontaining disks supported by a lifting mechanism, exposed to the air to capture CO2 during the adsorption phase. The disks are then lowered into a regeneration chamber for vacuum and steam regeneration to produce CO2 product during the desorption step. The modular tree design allows large installations with repeatable, mass-manufactured units connected to common utilities such as steam supply, vacuum, and CO2 processing for compression and geologic storage. The passive DAC system eliminates the equipment and energy of forced air fans by using natural air circulation to contact the sorbent with the CO2 in the air. Because of this, the performance is dependent on the wind speed in addition to the temperature and relative humidity. Performance and flow rate fluctuations were incorporated into equipment and facility design with considerations for turndown to 10% of maximum rated flow to allow operation in all seasons. The feasibility study was undertaken to evaluate the technology in different regions and climates. Three locations were selected for this study representing different climates: Alabama (hot and humid), California (hot and arid), and Wyoming (continental). For each region, the adsorption/desorption cycle was optimized including tuning the heat integration and cycle timings. The performance of individual trees was then scaled to the full facility with the same design of more than 20,000 trees common between all regions. The installations had expected average CO2 capture rates of between 330,000 and 485,000 tonnes of CO2 per year depending on the climate. The initial engineering design for the facility at each location was performed with cost and performance estimates for the trees, carbon purification and compression, and the balance of plant. To supply thermal and electrical energy for the facility, carbon-free or low-carbon power must be considered. Options for low-carbon, continuous thermal and electrical energy were considered. The best-performing option from those considered was identified to be an electrically-heated molten salt energy storage system, powered by an on-site photovoltaic field. During molten salt thermal discharge, steam is produced from heat exchange with the molten salt and used to generate power in a steam turbine as well as steam for regenerating the DAC carbon trees. The thermal and electrical supply and analysis is presented in the context of low-carbon power for carbon removal. Modelling and economics of transportation and geologic storage of the CO2 is considered and presented for each location. The results of the feasibility study are incorporated into the presented techno-economic and life-cycle assessments. This work is intended to provide an understanding of the performance, cost, and impact of capturing CO2 at the commercial scale and the impact of climate and regional siting on the considered passive DAC system.

42 ENGINEERING↗
DOE OSTI2025

CACTUS: CO 2 Aerogel Capture Towards Utilization and Sequestration

The CACTUS project aimed to develop a novel solid sorbent and sorption module prototype for direct air capture (DAC) of carbon dioxide, by a moisture-swing adsorption (MSA) mechanism. Because MSA uses changes in humidity, not temperature to switch the sorbent from capturing CO 2 to releasing concentrated CO 2 it is > 4X more energy-efficient than the thermal swing process. The goal was to develop a sorbent with a CO 2 capture capacity of 1 mmol CO 2 /g sorbent (or 0.75 mmol CO 2 /g structured sorbent), at a projected scaled cost of < $\$$15/kg sorbent and demonstration of a path to < $\$$100/ton CO 2 . At the end of the project, we achieved 0.8 mmol CO 2 /g sorbent powders, 0.37 mmol CO 2 /g structured sorbent (50% of target), at a projected cost of $\$$29/kg sorbent and an estimated cost of $\$$160/ton CO 2 . The key innovation was SRI’s patented polymer aerogel synthesis platform, which was adapted to produce a nanoporous aerogel with a high density of CO 2 -adsorbing quaternary ammonium groups. This research discovered a new ammonium polymer sorbent and identified a chemical path for its fabrication. The new process solved the monomer immiscibility challenge encountered with the initial method (ammonium is hydrophilic and the crosslinker is hydrophobic). The team fabricated structured sorbent sheets consisting of a non-woven porous substrate impregnated with ammonium polymer and demonstrated its operation in custom made breakthrough test setup MSA DAC built at SRI, and which operates similarly to the envisioned large-scale CO 2 capture plant, to provide data for techno-economic analysis (TEA). TEA sensitivity analysis indicated that ∼$\$$100/ton CO 2 can be achieved if the target capacity of 0.75 mmol CO 2 /g structured sorbent is met. Also identified routes to decrease sorbent manufacturing cost to ∼$\$$19/kg by reducing amounts and recycling the organic solvents. More work is needed on transitioning process manufacturing from powders (which showed a capacity of up to 0.8 mmol/g sorbent) to structured sheets which showed a capacity of 0.37 mmol CO 2 /g structured sorbent (or 0.44 mmol/g sorbent if one excludes the inert porous substrate). This is likely due to different micro/nano-structure of the sorbent and material processing constraints at the laboratory scale. Sorbent cycling studies (> 100 cycles) are needed to investigate its performance stability over time.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2024

Maximum and Comparative Efficiency Calculations for Integrated Capture and Electrochemical Conversion of CO 2

CO 2 as a C1 feedstock is receiving increasing attention, but it typically exists in dilute or impure streams. The capture and conversion of CO 2 to fuels or chemicals using carbon-neutral energy mitigates carbon emissions when CO 2 is captured from point sources and results in net or negative carbon emissions when CO 2 is obtained by direct air capture. Additionally, CO 2 capture and conversion steps are typically viewed as separate processes that optimize either capture and concentration or catalytic conversions of pure streams of CO 2 .

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

Multiscale Electricity Modeling for Evaluating Carbon Capture and Sequestration Technologies (Final Report)

Carbon capture and sequestration (CCS) technologies that can operate with a high degree of operating flexibility could provide necessary electric grid flexibility in a system with high shares of variable renewables. This project examines the deployment and dispatch potential of twelve unique flexible CCS (FLECCS) technologies that encompass post-combustion carbon dioxide (CO 2 ) capture designs, concepts using a storage media to enable energy arbitrage, and hybrid processes that integrate CCS with direct air capture (DAC) for flexibility with net zero or negative CO 2 emissions. FLECCS technology potential is explored with a multi-model, multi-scale framework including the Regional Energy Deployment System (ReEDS) electric sector capacity expansion model (CEM) and the PLEXOS production cost model (PCM). Innovative methods were developed to represent FLECCS technology operating modes, performance, and cost in the two models. ReEDS was then used to simulate nine scenarios for each FLECCS technology, three CO 2 emissions price futures reaching $\$$150, $\$$225, and $\$$300/tCO 2 in 2050; and three scenarios for FLECCS technology deployment favorability relative to competing technologies. For each CO 2 price and reference FLECCS favorability, the 2050 infrastructures from ReEDS model are downscaled and implemented in PLEXOS to examine hourly dispatch under detailed operational constraints that are not included in ReEDS. FLECCS technologies exhibited a wide range of deployment potential ranging from none to several hundred gigawatts of capacity, with outcomes highly sensitive to input cost and performance parameters that are inherently highly uncertain. When deployed, FLECCS tended to displace a combination of wind, solar, and natural gas-based technologies rather than supporting increased renewable deployment. As a result, CO 2 emissions reductions facilitated by FLECCS deployment tended to come with higher overall system costs and electricity prices. When economically competitive, FLECCS technologies can contribute significant flexible generation and firm capacity to the grid, but continued technology development and an expanded analytical scope are necessary to fully understand FLECCS deployment potential its impact on the electric power sector. Follow-on analysis incorporating captured CO 2 tax credit value from the Inflation Reduction Act (IRA) and other potential policy scenarios could be particularly valuable, as this policy can substantially change the relative competitiveness of FLECCS technologies.

03 NATURAL GAS↗
DOE OSTI2022

Catalytic Processes to Accelerate Decarbonization in a Net-Zero Carbon World

Reducing carbon dioxide emissions is one of the critical challenges to mitigate global climate change, which is having detrimental impacts on society and the environment. Fossil fuel combustion in transportation, power generation, and industrial processes is the dominant contributor to carbon emissions. Over the past decades, sustainable solutions and strategies have been investigated and developed to enable decarbonization. Catalysis plays an essential role to address this global challenge by increasing energy efficiency, reducing carbon emissions, capturing carbon dioxide, and utilizing clean energy sources to displace fossil fuels. In this Review, the role of catalysis in reducing energy demand was discussed, enhancing process efficiency, displacing carbon-intensive feedstocks and products, and therefore, reducing carbon emissions. Here, recent advances in catalyst development were summarized, focusing on applications to enhance industrial processes efficiency and enable utilization of clean energy sources. Emerging approaches in catalysis were reviewed, including the manufacture of iron and steel, direct air capture of CO 2 , production of ethylene, ammonia, and sustainable aviation fuels, plastic recycling, and the synthesis of biobased plastics. The Review was concluded with suggested research directions to achieve a carbon net-zero world.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Amine functionalized supported ionic liquid membranes (SILMs) for CO 2 /N 2 separation

Supported ionic liquid membranes (SILMs), containing aprotic N-heterocyclic anion ionic liquids (AHA ILs) in an inorganic inert support, exhibit CO 2 /N 2 permselectivity values as high as 640 at 35.0 °C and 0.03 bar CO 2 , which represents conditions similar to post-combustion carbon capture (PCCC) from a natural gas power plant. A Fickian model fit to the experimental data estimates CO 2 permeability at direct air capture (DAC) conditions of 10,400 barrer and a CO 2 /N 2 permselectivity of 4000 for the best performing IL, triethyl(octyl)phosphonium 4-bromopyrazolide ([P 2228 ][4-BrPyra]). The most important criterion for high selectivity is a large equilibrium constant for binding between the IL and CO 2 , which results in high CO 2 solubility. ILs with smaller molar volumes and with no fluoroalkyl chains enhance N 2 rejection. As a result, low viscosity and high IL molar density also enhance CO 2 /N 2 permselectivity and CO 2 permeance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Role of Intermolecular Interactions in Deep Eutectic Solvents for CO 2 Capture: Vibrational Spectroscopy and Quantum Chemical Studies

Recent research and reviews on CO 2 capture methods, along with advancements in industry, have highlighted high costs and energy-intensive nature as the primary limitations of conventional direct air capture and storage (DACS) methods. In response to these challenges, deep eutectic solvents (DESs) have emerged as promising absorbents due to their scalability, selectivity, and lower environmental impact compared to other absorbents. However, the molecular origins of their enhanced thermal stability and selectivity for DAC applications have not been explored before. Therefore, the current study focuses on a comprehensive investigation into the molecular interactions within an alkaline DES composed of potassium hydroxide (KOH) and ethylene glycol (EG). Combining Fourier transform infrared (FT-IR) and quantum chemical calculations, the study reports structural changes and intermolecular interactions induced in EG upon addition of KOH and its implications on CO 2 capture. Experimental and computational spectroscopic studies confirm the presence of noncovalent interactions (hydrogen bonds) within both EG and the KOH-EG system and point to the aggregation of ions at higher KOH concentrations. Additionally, molecular electrostatic potential (MESP) surface analysis, natural bond orbital (NBO) analysis, quantum theory of atoms-in-molecules (QTAIM) analysis, and reduced density gradient-noncovalent interaction (RDG-NCI) plot analysis elucidate changes in polarizability, charge distribution, hydrogen bond types, noncovalent interactions, and interaction strengths, respectively. Evaluation of explicit and hybrid models assesses their effectiveness in representing intermolecular interactions. This research enhances our understanding of molecular interactions in the KOH-EG system, which are essential for both the absorption and desorption of CO 2 . The study also aids in predicting and selecting DES components, optimizing their ratios with salts, and fine-tuning the properties of similar solvents and salts for enhanced CO 2 capture efficiency.

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

From Structured Solvents to Hybrid Materials (SS2HM) for Chemically Selective Capture and Electromagnetic Release of CO 2 : Mechanisms, Stability and Interfaces (Final Report)

The goal of this research program was to develop high capacity sorbents amenable for alternative regeneration approaches for direct air capture (DAC) of CO 2 . In particular, the research aimed to develop an understanding of CO 2 binding mechanism, thermal and oxidative stability, and regeneration energetics of functionalized ionic liquids (ILs), deep eutectic solvents (DESs), and porous materials. ILs and DESs are high-dielectric solvents with structural tunability that permits the rational-design for energy-efficient regeneration approaches based on electromagnetic (EM) field and moisture-swing. By further incorporating these solvents into polymeric capsules and other structural supports, multi-scale interfaces for targeted CO 2 and energy transfers were achieved. Aspects related to CO 2 capacity, selectivity, stability, dielectric properties, and binding energies were examined through experimental and computational design to identify molecular descriptors to inform future design of structured solvents and hybrid materials for DAC. Enclosed final report details the key findings, science advancements, and workforce development efforts from this project.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Sustainable Aviation Fuels from 30,000 feet – Scoping Report

A literature review, first principles analysis, and mapping of the airline-fuel infrastructure were performed to reassess the potential for various means of realizing a sustainable aviation sector. The literature review found a plethora of technical methods to make the airline industry net-zero CO 2 but limited work on the emergent barriers to sustainable aviation implementation such as land use, repurposing of fuel refining assets, and airline cost structures. First principles analyses of the energy, land, and costs of three broad net-zero strategies were performed to determine if sustainable aviation is feasible even in the most optimistic scenarios. Those methods were biomass-derived sustainable aviation fuel (SAF), fuel produced from CO 2 captured from the air and H 2 produced from water electrolysis (air-to-fuel: ATF), and offsetting fossil-derived Jet Fuel with carbon dioxide removal from the atmosphere (direct air capture and storage: DACS). Offsetting CO 2 emissions from using fossil Jet Fuel with DACS was found to consume the least energy, require the smallest quantity of land, and be the cheapest option. Replacing Jet Fuel with SAF was found to be only slightly more expensive than DACS but require substantially more land. ATF was found to be the most expensive and energy intensive option, though it did spare land relative to SAF. We found that calls to utilize waste biomass are well-founded, but wastes alone cannot cover the needs of the global airline industry. This means additional land will need to be allocated for biomass cultivation if SAF becomes the primary pathway to sustainable aviation. While differences were found in the performance of different types of biomass, those differences were small relative to differences with ATF and DACS. An analysis of the pricing structure of the airline industry suggests that some of the cost advantage of DACS may be erased by consumer sentiment which could explain why, to-date, the airline industry is focused primarily on SAF and to a lesser extent ATF. Further work is required to estimate the transportation, capital cost, and financing cost implications of greenfield and brownfield sites for SAF, DACS, and ATF. In the final report, we will analyze the potential to retrofit corn ethanol facilities to operate the ethanol-to-jet fuel process in response to decreasing gasoline demand as the electrification of road transport progresses. We will also construct a prioritization of land use to determine whether each net-zero CO 2 aviation pathway can make claim to the land required by their technology.

09 BIOMASS FUELS↗
DOE OSTI2024

FEED Study of Carbon Capture Inc. DAC and CarbonCure Utilization Using United States Steel's Gary Works Waste Plant

The University of Illinois Urbana-Champaign (UIUC) is spearheading a front-end engineering design (FEED) study of a Direct Air Capture and Utilization System (DACUS) that can remove 5,000 tonnes/yr net CO2 from ambient air, utilizing it in the production of concrete. The designed system, if built, would be larger than any currently existing DAC collector. Such carbon negative technologies are critical to meeting the goals of the DOE’s program to accelerate climate-critical technology. DAC is a promising new technology for reducing the greenhouse gas in the atmosphere but is expensive, partly due to the energy required to capture and then release CO2 during the process. By integrating CarbonCapture Technologies Inc. DAC collector at United States Steel's Gary Works and utilizing steel plant's waste heat, energy, and location so energy & transportation costs can be minimized. CarbonCapture has developed an innovative DAC system using novel adsorbents to cost- effectively capture CO2. The captured, liquified CO2 will be trucked to ready-mix concrete plants across Illinois, Indiana, & Wisconsin, where CarbonCure will inject it into concrete during the mixing process. The carbon dioxide reacts with concrete, mineralizing into calcium carbonate (CaCO3), sequestering the CO2 into the concrete, and reducing the amount of cement, the manufacturing of which is among the major sources of CO2 emissions. This FEED study demonstrates a full CO2 value chain for DACUS from industrial facilities. It also provided an opportunity to assess the impact of this holistic approach on job creation, regional economic impact, and environmental justice.

Carbon management, ccus, carbon capture, utilizati↗
DOE OSTI2024

Understanding the effect of density functional choice and van der Waals treatment on predicting the binding configuration, loading, and stability of amine-grafted metal organic frameworks

Metal organic frameworks (MOFs) are crystalline, three-dimensional structures with high surface areas and tunable porosities. Made from metal nodes connected by organic linkers, the exact properties of a given MOF are determined by node and linker choice. MOFs hold promise for numerous applications, including gas capture and storage. M2(4,4′-dioxidobiphenyl-3,3′-dicarboxylate)—henceforth simply M2(dobpdc), with M = Mg, Mn, Fe, Co, Ni, Cu, or Zn—is regarded as one of the most promising structures for CO2 capture applications. Further modification of the MOF with diamines or tetramines can significantly boost gas species selectivity, a necessity for the ultra-dilute CO2 concentrations in the direct-air capture of CO2. There are countless potential diamines and tetramines, paving the way for a vast number of potential sorbents to be probed for CO2 adsorption properties. The number of amines and their configuration in the MOF pore are key drivers of CO2 adsorption capacity and kinetics, and so a validation of computational prediction of these quantities is required to suitably use computational methods in the discovery and screening of amine-functionalized sorbents. In this work, we study the predictive accuracy of density functional theory and related calculations on amine loading and configuration for one diamine and two tetramines. In particular, we explore the Perdew–Burke–Ernzerhof (PBE) functional and its formulation for solids (PBEsol) with and without the Grimme-D2 and Grimme-D3 pairwise corrections (PBE+D2/3 and PBEsol+D2/3), two revised PBE functionals with the Grimme-D2 and Grimme-D3 pairwise corrections (RPBE+D2/3 and revPBE+D2/3), and the nonlocal van der Waals correlation (vdW-DF2) functional. We also investigate a universal graph deep learning interatomic potential’s (M3GNet) predictive accuracy for loading and configuration. These results allow us to identify a useful screening procedure for configuration prediction that has a coarse component for quick evaluation and a higher accuracy component for detailed analysis. Our general observation is that the neural network-based potential can be used as a high-level and rapid screening tool, whereas PBEsol+D3 gives a completely qualitatively predictive picture across all systems studied, and can thus be used for high accuracy motif predictions. We close by briefly exploring the predictions of relative thermal stability for the different functionals and dispersion corrections.

Chemistry↗
DOE OSTI2025

Surface-Enhanced Raman Detection of the CO 2 Moisture Swing

The development of scalable, energy-efficient carbon dioxide (CO 2 ) capture technologies is critical for achieving net-zero emissions. Moisture swing (MS) sorbents offer a promising alternative to traditional thermal regeneration methods by enabling reversible CO 2 binding through humidity-driven ion hydrolysis. In this study, we investigate the anion speciation dynamics in two classes of MS materials─an anion-exchange resin with a bicarbonate anion and activated carbon impregnated with potassium bicarbonate salt─using both sorption measurements and in situ surface-enhanced Raman spectroscopy (SERS). Ni-coated Ag nanowires were employed as SERS substrates to enhance signal intensity and enable the real-time detection of carbonate (CO 3 2– ), bicarbonate (HCO 3 – ), and hydroxide (OH – ) species under controlled humidity conditions in both air and nitrogen atmospheres. The results reveal humidity-dependent interconversion between anionic species with significant spectral shifts confirming the reversible hydrolysis reactions that drive the MS mechanism. Under humid conditions, we observed the depletion of bicarbonate signals and a concurrent increase in carbonate species, consistent with moisture-induced desorption of CO 2 . With the activated carbon samples, we further observed the formation of hydroxide. These findings not only validate the mechanistic models of humidity-driven anion exchange in MS sorbents but also demonstrate the practical potential of SERS as an operando diagnostic tool for monitoring CO 2 capture media. The ability to resolve and semiquantitatively evaluate the reversible transformation of carbonate, bicarbonate, and hydroxide ions under realistic environmental conditions provides valuable insight for the rational design, performance optimization, and quality control of next-generation sorbent materials for direct air capture applications.

CO2 capture↗
DOE OSTI2024

Light Water Reactor Sustainability Program: Technical and Economic Considerations for Uprate of Existing Nuclear Reactors with Cogeneration

The United States nuclear reactor fleet consists of 63 pressurized water reactors and 31 boiling water reactors and is a pivotal component in the nation's energy infrastructure, supplying approximately 97 GW e of clean power. With the country's commitment to decarbonization by 2050, these reactors are not only instrumental in decarbonizing the electricity grid but also play a critical role in decarbonizing industrial processes, producing clean fuels, and scaling up CO 2 removal. This report delves into the potential for power uprates in the existing fleet to contribute to these decarbonization efforts, focusing on the expansion of capacity for applications such as hydrogen production and carbon capture and sequestration. Building on previous research, the report explores regional market demands for hydrogen, oxygen, and carbon dioxide, financial implications of oxygen and CO 2 sales from high-temperature steam electrolysis systems, and the potential for direct air capture systems paired with uprated nuclear plants.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗