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At least 91 records · Page 5

Combining Eddy Covariance Towers, Field Measurements, and the MEMS 2 Ecosystem Model Improves Confidence in the Climate Impacts of Bioenergy With Carbon Capture and Storage

ABSTRACT Carbon dioxide removal technologies such as bioenergy with carbon capture and storage (BECCS) are required if the effects of climate change are to be reversed over the next century. However, BECCS demands extensive land use change that may create positive or negative radiative forcing impacts upstream of the BECCS facility through changes to in situ greenhouse gas fluxes and land surface albedo. When quantifying these upstream climate impacts, even at a single site, different methods can give different estimates. Here we show how three common methods for estimating the net ecosystem carbon balance of bioenergy crops established on former grassland or former cropland can differ in their central estimates and uncertainty. We place these net ecosystem carbon balance forcings in the context of associated radiative forcings from changes to soil N 2 O and CH 4 fluxes, land surface albedo, embedded fossil fuel use, and geologically stored carbon. Results from long term eddy covariance measurements, a soil and plant carbon inventory, and the MEMS 2 process‐based ecosystem model all agree that establishing perennials such as switchgrass or mixed prairie on former cropland resulted in net negative radiative forcing (i.e., global cooling) of −26.5 to −39.6 fW m −2 over 100 years. Establishing these perennials on former grassland sites had similar climate mitigation impacts of −19.3 to −42.5 fW m −2 . However, the largest climate mitigation came from establishing corn for BECCS on former cropland or grassland, with radiative forcings from −38.4 to −50.5 fW m −2 , due to its higher plant productivity and therefore more geologically stored carbon. Our results highlight the strengths and limitations of each method for quantifying the field scale climate impacts of BECCS and show that utilizing multiple methods can increase confidence in the final radiative forcing estimates.

Falvo, Grant [Department of Plant, Soil and Microb

Overcoming the Entropy Penalty of Direct Air Capture for Efficient Gigatonne Removal of Carbon Dioxide

Atmospheric carbon poses an existential threat to civilization via global climate change. Hundreds of gigatonnes of carbon dioxide must be removed from earth’s atmosphere in the next three decades, necessitating a low-cost, energy-efficient process to extract low concentrations of carbon dioxide for conversion to a stable material permanently stored for thousands of years. In this work, the challenge of removing gigatonnes of CO 2 is described via the scale of effort and the thermodynamics of collecting and reducing this diffuse chemical, the accumulation of which imparts a substantial entropy penalty on any atmospheric carbon capture process. The methods of CO 2 reduction combined with upstream direct air capture (DAC) including absorption, membrane separation, and adsorption are compared with biomass torrefaction and permanent burial (BTB). A Monte Carlo model assesses the mass, energy, and economics of the full process of biomass torrefaction from biomass collection and transport to stable carbon burial to determine that 95% of scenarios could remove carbon for less than $200 per CO 2 -tonne-equivalent. Torrefied carbon is further discussed for its long-term stability and availability at the scale required to substantially mitigate the threat of climate change.

biomass

Collaborative Approach to Identify Degradation Mechanisms and Validate Aging Protocols for a Diverse Set of DAC Materials (TCF Base Technology-Specific Final Report)

This work supports the mission of the U.S. Department of Energy to promote American energy leadership, technological innovation, and economic growth through the development of technologies for cost effective carbon capture. While capture technologies can provide carbon dioxide for enhanced oil recovery, many capture materials suffer from oxidative, hydrolytic and/or thermal degradation which leads to capacity loss and unwanted emissions such as ammonia. Short lifetimes increase operational costs and cost studies suffer from uncertainty because the true lifetimes of many capture materials are unknown. In this study, a suite of capture materials were studied to quantify their degradation, provide insight into the mechanisms that lead to their uptake loss and provide validated accelerated aging protocols for industry.

36 MATERIALS SCIENCE

Acoustic Emissions Sensing for Tracing Carbon Dioxide Movement in Caprock of a Carbon Capture Utilizations and Storage System (CCUS) (Final Technical Report)

The overall objective of this research project was to develop a non-invasive acoustic-emission (AE)-based technology that can accurately predict the location and movement of CO 2 through a confining layer in a carbon capture, utilization, and storage (CCUS) system. Specifically, the aim was to explore the feasibility of using the Haines jumps AEs as a passive method to track movement of CO 2 in reservoirs used for CCUS applications.

47 OTHER INSTRUMENTATION

New Molecular Mechanisms for Greenhouse Gas Capture in Metal-Organic Frameworks: Carbon Dioxide and Beyond

Separations involving gaseous small molecules, including acid gases, nitrous oxide, and hydrofluorocarbons, are vital to U.S. energy and technological dominance. However, many current separations technologies are too energy-intensive for broad deployment. Sorptive separations, in which a mixture of gases is contacted with a porous solid material, leading to separation based on the differing affinity of the gases for the solid, promise lower energy requirements compared to many existing technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Seawater alkalization via an energy-efficient electrochemical process for CO 2 capture

Electrochemical pH-swing strategies offer a promising avenue for cost-effective and energy-efficient carbon dioxide (CO 2 ) capture, surpassing the traditional thermally activated processes and humidity-sensitive techniques. The concept of elevating seawater’s alkalinity for scalable CO 2 capture without introducing additional chemical as reactant is particularly intriguing due to its minimal environmental impact. However, current commercial plants like chlor-alkali process or water electrolysis demand high thermodynamic voltages of 2.2 V and 1.23 V, respectively, for the production of sodium hydroxide (NaOH) from seawater. These high voltages are attributed to the asymmetric electrochemical reactions, where two completely different reactions take place at the anode and cathode. Here, we developed a symmetric electrochemical system for seawater alkalization based on a highly reversible and identical reaction taking place at the anode and cathode. We utilize hydrogen evolution reaction at the cathode, where the generated hydrogen is looped to the anode for hydrogen oxidation reaction. Theoretical calculations indicate an impressively low energy requirement ranging from 0.07 to 0.53 kWh/kg NaOH for established pH differences of 1.7 to 13.4. Experimentally, we achieved the alkalization with an energy consumption of 0.63 kWh/kg NaOH, which is only 38% of the theoretical energy requirements of the chlor-alkali process (1.64 kWh/kg NaOH). Further tests demonstrated the system’s potential of enduring high current densities (~20 mA/cm 2 ) and operating stability over an extended period (>110 h), showing its potential for future applications. Notably, the CO 2 adsorption tests performed with alkalized seawater exhibited remarkably improved CO 2 capture dictated by the production of hydroxide compared to the pristine seawater.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Integrated CO 2 Capture and Conversion to Formate with a Molecular Platinum Bis(diphosphine) Electrocatalyst

Carbon dioxide is a potentially valuable feedstock for carbon-based fuels or commodities but is only available in dilute streams. Many studies have focused on either the capture and concentration of CO 2 or the reduction of pure CO 2 streams. The direct reduction of sorbent-captured CO 2 in an integrated process would skip the energy-intensive CO 2 concentration and sorbent regeneration step. Herein, we report the electrocatalytic reduction of 1,3-bis(2,6-diisopropylphenyl)imidazolium-2-carboxylate (IPr·CO 2 ), which forms quantitatively from the reaction of sorbent 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene (IPr) with 10% and 0.04% CO 2 streams, by catalyst [Pt(dmpe) 2 ](PF 6 ) 2 (dmpe = 1,2-bis(dimethylphosphino)ethane) to formate with >70% Faradaic efficiencies. Unexpectedly, experimental studies indicate that the proton source phenol facilitates rapid decarboxylation of IPr·CO 2 to release CO 2 , which is the substrate for reduction. Kinetic studies determined the rate of hydride transfer from a catalytic intermediate [HPt(dmpe) 2 ](PF 6 ) to form the C–H bond in formate to be 0.22 M –1 s –1 . Further details on the mechanism, transition state energy, and structure for hydride transfer to CO 2 , a common step in CO 2 reduction, were explored using computational methods.

Chemistry

Enhanced Outcrop Methane Capture (Final Project Report)

This report provides the final status of the “Enhanced Outcrop Methane Capture (EOMC) Project” which was focused on drilling two new methane capture wells along the Fruitland Formation Outcrop for capture of methane and carbon dioxide which are naturally seeping from the Outcrop. The EOMC Project was focused on evaluating whether novel horizontal drilling technology will result in improved capture of methane and carbon dioxide which are naturally seeping from the Fruitland Formation Outcrop on Southern Ute tribal trust lands within the Southern Ute Indian Reservation (the “Reservation”).

01 COAL, LIGNITE, AND PEAT

Solid State Air Purification System

Life support systems in spacecraft are designed to provide a safe, habitable environment for the astronauts, and one of the most significant challenges is managing acceptable air quality. Carbon dioxide (CO2) is respired normally by humans at concentrations that are toxic if inhaled directly, and as a result cabin air must be tightly managed. The Carbon Dioxide Removal Assembly (CDRA) currently on board the ISS is the best functioning technology for manned space cabins, but has two significant drawbacks:1. The CDRA requires that air be dried prior to CO2 capture, and this costs energy _ in fact, the system spends 4X more energy drying the air than in actually capturing and releasing carbon dioxide. 2. The CDRA works in batch mode, while downstream CO2 processing systems require a continuous stream of CO2. This adds unnecessary complexity, as well as a second parasitic energy loss.An ideal system would process CO2 continuously without any need for drying of the air, and without any moving parts. Such a system would require a fraction of the size and weight of the CDRA while dropping the cost of CO2 capture by 5X or more. Such a technology would be enabling for future long term manned flight missions, such as a mission to Mars. eSionic is developing a new electrochemical membrane technology using its patented innovations in electrolyte materials. In Phase I of this program eSionic has demonstrated continuous gas separation using only electricity to drive the separation, with no moving parts or pressure drops. In Phase II, eSionic will demonstrate long-term operation of the membranes consistent with the needs of NASA for this development program.

Life Support

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

Optimizing Alabama’s CO 2 Storage in Shelby County (OASIS) (Final Report)

Optimizing Alabama’s CO 2 Storage in Shelby County (Project OASIS) is a CarbonSAFE Phase II designed to support the U.S. Department of Energy’s goals of reducing project risks and costs for future carbon dioxide (CO 2 ) capture, utilization, and storage (CCUS) projects, bringing more storage resources into commercial classifications that support business and financial decisions, and encouraging more rapid growth of a vibrant, geographically widespread industry for geologic carbon storage.

01 COAL, LIGNITE, AND PEAT

Carbon Capture Pilot at Vicksburg Containerboard Mill (Final Technical Report)

This is the final technical report for the DOE-OCED project DE-CD0000051. The report provides the progress at the close of the project. The objective of the project is to design and build a large pilot plant for carbon dioxide (CO 2 ) capture from a pulp and paper (P&P) mill using RTI’s non-aqueous solvent (NAS) technology at a capacity of 120,000 t-CO 2 /year, with >90% CO 2 captured. The pilot plant will be used for testing and evaluating the NAS capture process using real flue gas from the P&P mill’s power boiler for a minimum of 1 year of parametric testing and a minimum of 2,000 hours of continuous long-term testing. The testing will provide data for process optimization and scale-up for the P&P industry, provide information on interaction of flue gas contaminants on solvent performance and degradation, and inform strategies for emission control. At the end of the project, the pilot plant will be managed by International Paper (IP), the host site owner, which will continue to capture CO 2 , sequester the captured CO 2 , and be eligible for the 45Q credit.

42 ENGINEERING

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

Direct Air Capture and Electromicrobial Production (DAC-EMP) (Final Technical Report for ARPA-E Project)

The collaborative effort of UC Berkeley and GE Vernova (formerly GE Research) aimed to develop an integrated, three-step process to directly capture and convert carbon dioxide (CO 2 ) from ambient air into butanol, a platform molecule for diesel and jet fuels. This new process is intended to address the unmet need for carbon-neutral drop-in substitutes for fossil gasoline, which would substantially reduce the carbon footprint of the transportation sector without requiring significant changes to the nation’s transportation infrastructure. The U.S. alone consumes ~120 billion gallons of gasoline per year, and the use of fossil fuels in transportation accounts for ~30% of U.S. greenhouse gas emissions, a major contribution to the ongoing climate crisis. A successful replacement fuel must therefore be produced in a process that has low carbon emissions over its life cycle while demonstrating both scalability and economic competitiveness. The proposed system is tailorable to a wide range of applications and can establish a viable approach for direct capture and conversion of CO 2 to value-added products with much lower land use compared to a biotechnological process relying on corn-derived glucose.

09 BIOMASS FUELS

Iron Impurity Impairs the CO 2 Capture Performance of MgO: Insights from Microscopy and Machine Learning Molecular Dynamics

Magnesium oxide (MgO) is a promising sorbent for direct air capture (DAC) of carbon dioxide. Iron (Fe) is a common impurity in naturally occurring MgO and minerals used to produce MgO, yet a molecular-scale understanding of Fe-doping effects on carbonation is lacking. Here, in this study, we observed reduced carbonation performance in Fe-doped MgO experimentally. The energetics of adsorbing a (bi)carbonate ion on pristine and Fe-doped MgO(001) surfaces were further investigated using ab initio and machine learning potential molecular dynamics coupled with metadynamics simulations. Both pristine and Fe-doped surfaces exhibited a basic (OH – ) hydration layer, where the (bi)carbonate ion adsorption is thermodynamically favorable. However, the dissolution of surface Fe had smaller energy barriers and was more favorable than Mg. Leached Fe likely neutralized the near-surface basicity, yielding reduced reactivity on Fe-doped MgO. Our observations offer critical insights for material selection and emphasize the importance of evaluating the geologic origin of earth materials used for DAC.

36 MATERIALS SCIENCE

Integration of the fundamental knowledge on solvent-packing interactions into the multiscale framework for column scale design and optimization

The interfacial area, also known as the effective mass transfer area, is a key factor for determining the mass transfer for carbon dioxide (CO 2 ) capture via the chemical absorption process in a packed column, and thus the overall capture efficiency of the packed column. Most of the widely used empirical and semi-empirical models for interfacial area were derived indirectly through absorption mass transfer with simplifications based on fast chemical kinetics. This report presents the comprehensive unique multiscale approach to develop a surrogate model for effective mass transfer area in structured packed columns that accounts local hydrodynamics as well as variation in physical properties, and changes in solid surface characteristics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Comprehensive structural characterization of charged polymers involved in moisture-driven direct air capture

This study provides a comprehensive structural characterization of commercially available alkaline anion-exchange polymers (Fumasep FAA-3 and IRA 900) used in moisture-driven direct air capture (DAC) of carbon dioxide. Using X-ray diffraction, SAXS/WAXS, atomic force microscopy, FIB-SEM, and transmission electron microscopy, the authors identify nanoscale clustering, porosity, swelling behavior, and humidity-dependent structural changes that influence CO₂ adsorption and release. These findings establish structure–function relationships critical for designing more durable and energy-efficient DAC polymer materials.

36 MATERIALS SCIENCE

Atomistic Insights into the Reactive Diffusion of CO 2 in Guanidine-Based Facilitated Transport Membranes

The pressing need to address climate change has led to significant advancements in carbon dioxide (CO 2 ) capture technologies. Notably, facilitated transport membranes (FTMs) are distinguished by their exceptional selectivity and permeance, attributed to their reversible chemical reactions with CO 2 . This study, for the first time, sheds light on the reactive diffusion mechanism of CO 2 in FTMs, utilizing 1,1,3,3-tetramethylguanidine (TMG) as a mobile carrier. Specifically, state-ofthe- art molecular dynamics (MD) simulations, augmented by a reparameterized reactive force field (ReaxFF) capable of describing atomistic interactions and reaction pathways, are conducted to investigate the transport of CO 2 in TMG. The analysis of mean squared displacement (MSD) and diffusion coefficients reveals a clear hierarchy in the mobility of reaction components. Our findings highlight a unique hopping diffusion mechanism between bicarbonate ions and TMG molecules, increasing the diffusivity of reacted CO 2 by 1.4 times. The hopping events observed not only enhance our understanding of molecular mobility but also offer a means to boost the performance of FTMs in CO 2 capture applications. Overall, this research lays the groundwork for the future design of FTMs with optimal carrier properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH