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Vanadium peroxide molecules undergo stoichiometric direct air capture of carbon dioxide, wherein reactivity towards carbon capture via both peroxide and adventitious superoxide ligands trends with the size of the alkali countercation.
Direct air capture (DAC) of carbon dioxide is one approach among many proposed that is capable of offsetting hard-to-avoid emissions. In previous work, we developed the alkalinity concentration swing (ACS) method, which is driven through concentrating an alkaline solution that has been loaded with atmospheric CO 2 by desalination technologies, such as reverse osmosis or capacitive deionization. Though the ACS is promising in terms of energy usage and implementation, its absorption rate and water requirements are infeasible for a large-scale DAC process. Here, we propose an improvement on the ACS, the bicarbonate-enriched alkalinity concentration swing (BE-ACS), which selects bicarbonate ions from a stream of aqueous alkaline solution that has absorbed atmospheric CO 2 . The bicarbonate-rich stream is then concentrated, which greatly increases its CO 2 partial pressure, and then CO 2 is extracted from solution. We experimentally investigate the use of pressure-driven nanofiltration (NF) membrane-based separation to select bicarbonate ions over carbonate ions. We screen commercial membranes and select one high-performance membrane for detailed studies, quantifying its bicarbonate-carbonate selectivity factor and bicarbonate-passage factor. Feed pH, the combined concentration of aqueous CO 2 , bicarbonate, and carbonate species (or dissolved inorganic carbon), alkalinity, and permeation flux are systematically varied to study NF separation properties. We find that the selectivity factor, which exceeds 30 times in certain regimes, increases with higher feed pH and higher alkalinity. Lastly, the performance metrics of the selected NF membrane are input into a theoretical BE-ACS cycle analysis, and the required energy input and cycle capacity output are evaluated. Ideal cycle energy is found to be as low as around 250 kJ/mol, with opportunities identified for further decreases through process engineering and forward osmosis energy recovery.
Direct air capture (DAC) systems often consist of packing material wetted by a capture fluid that reacts with CO 2 in the airstream. The efficiency of the contactor is determined by a complex relationship of fluid dynamics, heat and mass transfer, contactor geometry, and chemical properties. The efficiency of the contactor must be balanced with other factors, primarily pressure drop through the system. Triply periodic minimal surfaces (TPMS) are a class of differential surfaces that have been explored in multiple engineering applications and have been shown to exhibit excellent performance when used in heat exchangers. Their tortuous path provides a high surface-to-volume ratio and favorable trade-off between contact area and pressure drop. In this work, a gyroid-type TPMS contactor was evaluated using computational fluid dynamics for a variety of geometric parameters to explore the potential benefit of TPMS shapes for DAC applications. A thin-film model was employed to model the flow and distribution of the capture solvent, allowing efficient simulations of TPMS structures at scale by eliminating the need for a computationally intensive interface capturing method. A liquid-gas mass transfer model was implemented in the commercial software STAR-CCM+ and used to predict the CO 2 capture efficiency and study the trade-off between capture performance and pressure drop through analysis of capture rates, mass transfer coefficients, and other relevant variables. TPMS contactors with a variety of geometric parameters and two capture solvent options were investigated to determine the effect of design choices on the operational performance of DAC systems. In conclusion, results showed that while contactor geometry is the dominant factor in efficiency and pressure drop, the physiochemical properties of the solvent are an important secondary influence on the contactor performance.
Carbon capture is essential to meeting climate change mitigation goals. One approach currently being commercialized utilizes liquid-based solvents to capture CO 2 directly from the atmosphere but is limited by slow absorption of CO 2 into the liquid. Improved air/solvent liquid mixing increases CO 2 absorption rate, and this increased CO 2 absorption efficiency allows for smaller carbon capture systems with lower capital costs and better economic viability. In this project, we study the use of passive micromixers fabricated by metal additive manufacturing. The micromixer’s small-scale surface geometric features perturb and mix the liquid film to enhance mass transfer and CO 2 absorption. In this project, we evaluated this hypothesis through computational and experimental studies. Computational investigations focused on developing capabilities to simulate thin film (~ 100μm) fluid flow on rough surfaces. Such thin films are in a surface-tension dominated regime and simulations in this regime are prone to instabilities. Improvements to the Nalu code completed in this project resulted in a 10x timestep stability improvement for these problems.
Limiting the rise in global temperature to 1.5 °C will rely, in part, on technologies to remove CO 2 from the atmosphere. However, many carbon dioxide removal (CDR) technologies are in the early stages of development, and there is limited data to inform predictions of their future adoption. Here, we present an approach to model adoption of early-stage technologies such as CDR and apply it to direct air carbon capture and storage (DACCS). Our approach combines empirical data on historical technology analogs and early adoption indicators to model a range of feasible growth pathways. We use these pathways as inputs to an integrated assessment model (the Global Change Analysis Model, GCAM) and evaluate their effects under an emissions policy to limit end-of-century temperature change to 1.5 °C. Adoption varies widely across analogs, which share different strategic similarities with DACCS. If DACCS growth mirrors high-growth analogs (e.g., solar photovoltaics), it can reach up to 4.9 GtCO 2 removal by midcentury, compared to as low as 0.2 GtCO 2 for low-growth analogs (e.g., natural gas pipelines). For these slower growing analogs, unabated fossil fuel generation in 2050 is reduced by 44% compared to high-growth analogs, with implications for energy investments and stranded assets. Residual emissions at the end of the century are also substantially lower (by up to 43% and 34% in transportation and industry) under lower DACCS scenarios. The large variation in growth rates observed for different analogs can also point to policy takeaways for enabling DACCS.
Direct air capture (DAC) of CO 2 is a promising solution for reducing the carbon footprint through "negative emission" technology. However, the low CO 2 concentration (~400 ppm) and the dynamic nature of DAC processes present challenges in designing effective sorbent systems. Recent advancements in material design and structural engineering have led to the development of high-performance solid sorbents, offering a more stable, safe, and energy-efficient alternative to traditional liquid CO 2 capture methods. This review highlights progress in solid sorbent-based DAC, focusing on amine-modified materials, hydrogen-bonded frameworks, and ionic liquid-engineered scaffolds. The discussion covers design principles, synthesis methodologies, and their impact on CO 2 chemisorption, comparing the advantages and limitations of each approach. Characterization techniques, especially operando methods and computational tools, are reviewed to understand sorbent behavior during CO 2 integration and release. The reaction pathways and interaction mechanisms of these sorbents with CO 2 are analyzed to guide future design. Additionally, the CO 2 chemisorption behaviors, including capacity, sorption kinetics, recyclability, and durability in the presence of gaseous impurities and under humid conditions will be evaluated and compared. Further, the review offers unique insights into the physical properties, chemical structures, and surface engineering effects of these sorbents, based on comprehensive characterization and evaluation techniques.
A techno-economic and environmental life cycle assessment was conducted for manufacturing two novel types of solid sorbents used for direct air CO 2 capture (DAC). One type of solid sorbent comprised Polyacrylonitrile (PAN)/Organopolysilizane (OPSZ)/nanoscale organic hybrid materials (NOHM)(, and the other comprised polymers of intrinsic microporosity (PIM)/NOHM. These solid sorbents were assumed to be manufactured via an unconventional route: electrospinning as fibers. Economic analyses revealed that manufacturing costs for a 0.73 MT/year capacity plant was $\$$831 and $\$$1398/kg of electrospun fiber in the case ofPAN/OPSZ/NOHM and PIM/NOHM, respectively. The costs were higher for PIM/NOHM owing to high raw material prices (Spirobisindane and tetrafluoroterephthalonitrile), that are used only in manufacturing PIM. Scaling up the plant capacity from 0.73 to 30 MT/year plant decreased the manufacturing cost by nearly half from $\$$831 to $\$$379 in the case of PAN/OPSZ/NOHM, depicting the economies of scale of effect. An LCA of both types of solid sorbent was performed using OpenLCA software, the Ecoinvent v 3.5 database, and the TRACI LCI assessment method. The Global Warming Potential (GWP) ofPAN/OPSZ/NOHM and PIM/NOHM was observed to be 151 × 10 -3 and 166 × 10 -3 kg CO 2 per kg CO 2 captured in the DAC plant, respectively. In conclusion, these GWP values were nearly five times as high as those observed for other solid sorbents existing in the literature such as PEI on silica gel, carbonate on silica, and carbonate on activated carbon owing to large amounts of electricity used in electrospinning unit operation.
The Palo Alto Research Center (PARC) developed a novel CO 2 adsorbent material, and in collaboration with Lawrence Livermore National Laboratory (LLNL), demonstrated its state-of-the-art performance for direct air capture. The target application for this technology is in direct air carbon capture and storage (DACCS), for which the adsorbent material provides the critical function of binding CO 2 from ambient air. At the beginning of the project, the technology concept and application were established, representing technology readiness level (TRL) 2. The hypothesis was that a microporous polymer comprising a high density of primary amines would make an exceptional adsorbent for direct air capture, and the goal of the project was to prove that hypothesis and advance the technology to TRL 3. To accomplish this, we approached the challenge from the perspective of materials synthesis optimization with the narrow focus of achieving the target material properties. This approach was successful, and we now have a synthetic procedure that results in a novel adsorbent material with the target material properties. The chemical name for the novel adsorbent material is poly(vinylamine-co-divinylbenzene) (PVAm-DVB).
Carbon Collect Inc., along with Arizona State University, the Electric Power Research Institute (EPRI), PM Group, and Trimeric Corporation, completed an initial design of a commercial-scale, passive direct air capture (DAC) system termed “carbon trees” that will capture, separate, and store at least 100,000 tonnes/year of carbon dioxide (CO2) from air (net basis). Passive DAC is unique among DAC technologies in that passive air delivery by wind avoids the energy penalty of forced convection. Carbon Collect Inc.’s sorbent-agnostic approach offers the flexibility to choose sorbents for a wide range of climates. A combination of steam, low-grade heat, and vacuum releases the CO2 from the sorbent, which is extracted from the chamber and purified and compressed for geological storage. A commercial carbon tree forest combines the output of several thousand trees for compression and purification with high heat and energy integration. The project team prepared an initial engineering design package for each of three geographically diverse host sites throughout the United States to better understand the effect of local/regional ambient conditions on DAC system performance and project costs. A techno-economic analysis, life cycle analysis, business case analysis, and an environmental, health, and safety risks assessment were also completed for each of the three geographically diverse host sites.
Correction for ‘Acid–base concentration swing for direct air capture of carbon dioxide’ by Anatoly Rinberg and Michael J. Aziz, Energy Adv. , 2024, https://doi.org/10.1039/d4ya00251b.
This final report, which is for DOE Award Number DE-FE0032160 (Direct Air Capture Combined with dedicated Long-Term Carbon Storage, Coupled to Existing Low-Carbon Energy), covers the Nuclear Direct Air Capture with Carbon Storage (NuDACCS) project period of performance from 03/31/2022 to 12/27/2024. Battelle Memorial Institute (Battelle) partnered with Aircapture LLC (Aircapture), Southern Company (Southern), Carbonvert, the University of Alabama, and Sargent & Lundy (S&L) to develop a front end engineering design (FEED) study for a direct air capture (DAC) system co-located with Southern Company's Joseph M. Farley Nuclear Plant (Plant Farley) in Columbia, Alabama. The DAC system was designed to capture at least 5,000 net tonnes of carbon dioxide (CO2) per year from ambient air in a form suitable for long duration carbon storage (e.g., geologic storage). To complement and support the FEED study, additional analyses were completed, including a Technology Maturation Plan (TMP); Workforce Readiness Plan; Project Cost Estimate; Business Case Analysis (BCA); Life Cycle Analysis (LCA); Environmental Health and Safety (EH&S) Assessment; and Environmental Justice (EJ) Analysis and Economic Revitalization and Job Creation Outcomes Analysis.
Direct air capture (DAC) is a growing field responding to the need to remove carbon dioxide from the atmosphere. Several technologies are being developed today attempting to meet this need. The technology furthest in development are temperature swing adsorption technologies which have recently moved out of the pilot plant scale.1 This presentation looks to present an electrochemical device as alternative to these technologies. The electrochemical device proposed is a pair of nickel hydroxide (Ni(OH)2) battery electrodes which produce hydroxide (OH-). The hydroxide reacts with carbon dioxide (CO2) to create carbonate (CO32-) and bicarbonate (HCO3-). These carbonates can be transported from the cathode across an anion exchange membrane to the anode where they are evolved back into CO2 due to a pH reduction at the anode. This builds on work that optimized a Hydroxide Exchange Membrane Fuel Cell (HEMFC) for CO2 capture, showing the efficacy of an electrochemically mediated pH swing carbon capture device.2,3 The benefit of the nickel hydroxide battery approach is the low energy cost associated with separation. Because a pair of nickel hydroxide batteries undergo the same electrochemical reaction, low potentials, and thus low energy cost is required. Experiments have shown device level energy requirements of less than 1 MWh ton-1CO2. Most of the energy required by the device produces the pH gradient used to capture and release CO2. The biggest hurdle for this electrochemical approach is increasing the flux of CO2 to allow for more compact devices. Strategies for managing the transient charge and discharge behavior of the battery system will be discussed. Focus will be on improving flux to reduce the overall cost of the device.
The overall objective of this project was to complete an initial design of a commercial-scale, Carbon Capture and Storage system for Direct Air Capture (CCS-DAC) that separates and stores a minimum of 100,000 tonnes/year (t/yr.) net CO 2 from air. Three geographically diverse host sites will be used to determine the impact of different climates on the design and cost of the CCS-DAC systems; California (dry-hot), Louisiana (humid-hot), and Wyoming (mid-continental). In addition, the impact of using different low-carbon energy sources was also examined. The focus of this project was to geologically store the CO 2 , rather than the utilization of CO 2 . This Final Scientific/Technical Report is a collection of the deliverables for the project. The project team was able to successfully complete all the necessary tasks needed to determine the feasibility of the designs and operational needs of the DAC systems for each location. The data created by this allowed the project team to conduct the required evaluations to meet the requirements of the deliverables. The following deliverables were drafted and submitted to DOE prior to the conclusion of the project: (1) Initial Engineering Design; (2) Costing Estimate; (3) Techno-Economic Analysis (TEA); (4) Life Cycle Analysis (LCA); (5) Business Case Assessment; and (6) Technology EH&S Risk Assessment.
This study investigates the development and economic analysis of a modular integrated system for carbon-neutral methanol synthesis, leveraging direct air capture (DAC) and solid oxide electrolysis cells (SOEC) for carbon dioxide and hydrogen production, respectively. The proposed system integrates a novel building-based DAC process, functionalized solid sorbents, and low-energy SOEC technology, aiming to minimize operational and capital costs. A comparison between the base case system (1,000 t methanol/year) and a scaled-up model (14,758 t methanol/year) reveals significant improvements in efficiency and economic feasibility. The scaled-up system achieves a levelized cost of methanol (LCOM) of $740/t, a 7.5% reduction compared to that of conventional DAC-based systems, while utilizing existing building HVAC infrastructure for air handling. Detailed sensitivity analyses were conducted, evaluating the effects of plant capacity and air flow rate on the LCOM, demonstrating the scalability of the building-based DAC system. The cradle-to-gate life cycle analysis shows that the proposed process using renewable-sourced electricity achieves a 38% reduction in greenhouse gas (GHG) emission compared to reported values of green methanol production technologies that use a conventional DAC and a conventional methanol synthesis catalyst. When fossil-sourced electricity is used in the proposed process, it leads to about a 37.5% reduction in GHG emission in comparison to reported values for conventional methanol production technologies using steam methane reforming technology and fossil-sourced electricity.
This work demonstrates the first experimental evidence of the acid–base concentration swing (ABCS) for direct air capture of CO 2 . This process is based on the effect that concentrating particular acid–base chemical reactants will strongly acidify solution, through Le Chatelier's principle, and result in outgassing absorbed CO 2 . After collecting the outgassed CO 2 , diluting the solution will result in a reversal of the acid–base reaction, basifying the solution and allowing for atmospheric CO 2 absorption. The experimental study examines a system that includes sodium cation as the alkalinity carrier, boric acid, and a polyol complexing agent that reversibly reacts with boric acid to strongly acidify solution upon concentration. Though the tested experimental system faces absorption rate and water capacity limitations, the ABCS process described here provides a basis for further process optimization. A generalized theoretical ABCS reaction framework is developed and different reaction orders and conditions are studied mathematically. Higher order reactions yield favorable cycle output results, reaching volumetric cycle capacity above 50 mM for third-order and 80 mM for fourth-order reactions. Optimal equilibrium constants are determined in order to guide alternative chemical searches and synthetic chemistry design targets. There is a substantial energetic benefit for reaction orders above the first, with second- and third-order ABCS cycles exhibiting a thermodynamic minimum work for the concentrating and outgassing steps around 150 kJ per mole of CO 2 . A significant advantage of the ABCS is that it can be driven through well-developed and widely-deployed desalination technologies, such as reverse osmosis, with opportunities for energy recovery when recombining the concentrated and diluted streams, and extraction can occur directly from the liquid phase upon vacuum application.
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Abstract Understanding the oxidative and thermal degradation of CO 2 sorbents is essential for assessing long‐term sorbent stability in direct air capture (DAC). The potential degradation pathway of imidazolium cyanopyrrolide, an ionic liquid (IL) functionalized for superior CO 2 capacity and selectivity, is evaluated under accelerated degradation conditions to elucidate the secondary reactions that can occur during repetitive absorption‐desorption thermal‐swing cycles. The combined analysis from various spectroscopic, chromatographic, and thermal gravimetric measurements indicated that radical and S N 2 mechanisms in degradation are encouraged by the nucleophilicity of the anion. Thickening of the liquid and gas evolution are accompanied by 50 % reduction in CO 2 capacity after a 7‐day exposure to O 2 under 80 °C. To prevent long exposure to conventional thermal heating, microwave (MW) regeneration of the CO 2 ‐reactive IL is used, where dielectric heating at 80 and 100 °C rapidly desorbs CO 2 and regenerates the IL without any measurable degradation.
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.