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Synthetic pathway for biological carbon dioxide sequestration
This invention relates to methods for increasing carbon fixation and/or increasing biomass production in a plant, comprising: introducing into a plant, plant part, and/or plant cell heterologous polynucleotides encoding (1) a succinyl CoA synthetase, (2) a 2-oxoglutarate:ferredoxin oxidoreductase, (3) a 2-oxoglutarate carboxylase, (4) an oxalosuccinate reductase, or (5) an isocitrate lyase, or (6) a succinyl CoA synthetase and a 2-oxoglutarate:ferredoxin oxidoreductase, (7) a 2-oxoglutarate carboxylase and an oxalosuccinate reductase polypeptide, and/or (8) a 2-oxoglutarate carboxylase polypeptide, an oxalosuccinate reductase polypeptide and an isocitrate lyase polypeptide to produce a stably transformed plant, plant part, and/or plant cell, wherein said heterologous polynucleotides are from a bacterial and/or an archaeal species. Additionally, transformed plants, plant parts, and/or plant cells are provided as well as products produced from the transformed plants, plant parts, and/or plant cells.
Mobilization of trace metals from caprock and formation rocks at the Illinois Basin – Decatur Project demonstration site under geological carbon dioxide sequestration conditions
One concern for geologic CO 2 sequestration is the potential leakage of CO 2 or CO 2 -saturated brine containing trace metals into overlying aquifers, which poses the risk of adversely affecting underground sources of drinking water. In this work, rock and brine samples collected in the Illinois Basin – Decatur Project (IBDP), a large-scale geological CO 2 sequestration demonstration project in Decatur, Illinois, USA, as well as synthetic brine samples were used to understand the mobilization of trace metals as a result of CO 2 –rock–brine interactions under IBDP-specific conditions (50 °C and 20.6 MPa). Rock sample characterization indicated that, at the IBDP site, trace metal concentrations were greatest in cap rock samples from the Eau Claire Formation, compared with those from formations above and below this Formation. The natural brine samples collected from the Mt. Simon Sandstone reservoir were highly reducing and saline, with trace metal concentrations up to 680 times greater than the U.S. Environmental Protection Agency-prescribed drinking water standards. Batch leaching experiments indicated that both trace metal mobilization from rock and immobilization from the brine occurred when high-pressure CO 2 was introduced into the rock-brine system. The amounts of metals mobilized from the rock generally accounted for <5% of the total metals in the rock, but for some metals, including Ni, Pb, and Tl, up to 63% of the metals in the rock were mobilized to the brine. Leaching of trace metals into synthetic brines was different from that into the natural brine. The results of this study provided current information on the trace element sources and will help in risk simulations and experimental design to further evaluate potential impact of leakage on groundwater quality, which is important for future GCS projects to consider for monitoring and containment assurance purposes.
Two novel Patescibacteria: Phycocordibacter aenigmaticus gen. nov. sp. nov. and Minusculum obligatum gen. nov. sp. nov., both associated with microalgae optimized for carbon dioxide sequestration from flue gas
The functional roles of bacterial symbionts associated with microalgae remain understudied despite the importance of microalgae in biotechnology and environmental microbiology. 16S rRNA gene sequencing was conducted to analyze bacterial communities associated with two microalgae optimized for growth with flue gas containing 5%–10% CO 2 . Two dominant bacteria with no taxonomic classification beyond the class level (Paceibacteria) were discovered repeatedly in the most productive algal cultures. Long-read metagenomic sequencing was conducted to yield high-quality metagenomes, from which two novel species were discovered under the Seqcode (seqco.de/r:ywe1blo2), Phycocordibacter aenigmaticus gen. nov. sp. nov. and Minusculum obligatum gen. nov. sp. nov. The genus Phycocordibacter gen. nov. was proposed as the nomenclatural type of the family Phycocordibacteraceae fam. nov. and the order Phycocordibacterales ord. nov. Both bacteria possessed features typical of Patescibacteria such as reduced genomes (<800 kbp), lack of complete glycolysis and tricarboxylic acid (TCA) cycle pathways, and inability to synthesize amino acids. Instead, they rely on the reductive pentose phosphate pathway (Calvin cycle) for essential biosynthesis and redox balance. P. aenigmaticus may also rely on elemental sulfur oxidation (sdo), partial nitrite reduction (nirK), and sulfur-related amino acid metabolism (SAMe → SAH). Both bacteria were found in high relative abundance in cultures of Tetradesmus obliquus HTB1 (freshwater) and Nannochloropsis oceanica IMET1 (marine), suggesting a tight association with microalgae in various environments. The absence of full metabolic pathways for energy production suggests extreme metabolic limitations and obligate symbiosis, most likely with other bacteria associated with the microalgae.
Geochemical assessment of mineral sequestration of carbon dioxide in the midcontinent rift
Abstract This study examines the potential of Midcontinent Rift rocks to facilitate long‐term CO 2 sequestration by providing the necessary Ca and Mg for carbonate mineralization. Surface samples were collected from the Oronto and Bayfield‐Jacobsville Groups around Lake Superior and used for petrography and X‐ray diffraction to determine their mineral composition. Also, X‐ray fluorescence was also used to assess their bulk chemical composition. The samples were then exposed to CO 2 and deionized water in Teflon‐lined vessels at 90°C, and the resulting leachate fluids were analyzed for the cation released during the testing. SEM microscopy was used to examine the samples for potential mineralization of carbonate minerals. The Oronto Group sediments consist primarily of feldspathic to feldspathic lithic arenites with a chlorite‐dominated matrix, and the primary porosity is blocked by calcite and hematite cement. The Bayfield–Jacobsville sequences are porous quartz arenites to feldspathic quartz arenites that do not contain significant accumulation of Ca‐, Mg‐, and Fe‐bearing minerals. The leachate fluids obtained from Oronto Group samples exhibit a maximum Ca release rate (5.2 × 10 −4 mole/cm 2 .day), indicating rapid calcite cement dissolution and increased porosity and permeability. SEM/EDS microanalysis revealed areas where pore‐filling calcite was preferentially dissolved. Longer‐term rock‐water reactions resulted in induced carbonate mineralization, as evidenced by calcite crystals observed in a sample reacted for 102 days. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
Local structure and distortions of mixed methane-carbon dioxide hydrates
A vast source of methane is found in gas hydrate deposits, which form naturally dispersed throughout ocean sediments and arctic permafrost. Methane may be obtained from hydrates by exchange with hydrocarbon byproduct carbon dioxide. It is imperative for the development of safe methane extraction and carbon dioxide sequestration to understand how methane and carbon dioxide co-occupy the same hydrate structure. Pair distribution functions (PDFs) provide atomic-scale structural insight into intermolecular interactions in methane and carbon dioxide hydrates. We present experimental neutron PDFs of methane, carbon dioxide and mixed methane-carbon dioxide hydrates at 10 K analyzed with complementing classical molecular dynamics simulations and Reverse Monte Carlo fitting. Mixed hydrate, which forms during the exchange process, is more locally disordered than methane or carbon dioxide hydrates. The behavior of mixed gas species cannot be interpolated from properties of pure compounds, and PDF measurements provide important understanding of how the guest composition impacts overall order in the hydrate structure.
Method for carbon dioxide capture and sequestration using alkaline industrial wastes
A method of sequestering gaseous carbon dioxide in which an oxide is carbonated by contacting it with a first aqueous carbonate solution to convert a portion of the oxide into a carbonate, which precipitates from solution. By converting the oxide to a solid carbonate, the CO 2 from the first carbonate solution is sequestered into the precipitate. At the same time, an aqueous hydroxide solution is formed. The aqueous hydroxide solution is contacted with gaseous carbon dioxide which sequesters the gaseous CO 2 into a second aqueous carbonate solution. The second solution so generated is then recycled back into the process and used to convert the oxide into the precipitated carbonate.
Gas Hydrate Film Growth in Microfluidic Channels for Carbon Dioxide Capture and Sequestration Applications
Gas or clathrate hydrates are a solid, crystalline compound composed of water and guest molecules that typically form at high pressure and low temperature conditions. Carbon dioxide (CO2) hydrates may be involved in several carbon dioxide capture and sequestration (CCS) applications, including CO2 pipeline transportation and CO2 offshore sequestration. Within these applications, the formation mechanism and kinetics must be well understood to manage the CCS processes, either by preventing or promoting hydrate formation. In this work, a high-pressure glass microfluidic reactor is used in tandem with visual microscopy and in-situ Raman spectroscopy to study both the morphological and kinetic behavior of gas hydrate crystals. Subcooling, pressure, and CO2 flow rate are investigated for their impact on the thickening behavior of pure CO2 hydrates, with flow rate being the only parameter to have a significant effect. Visual and Raman spectroscopy evidence show that both a dense hydrate layer and a porous hydrate layer form, and the latter may provide a path for mass transfer to continue hydrate crystallization. A first principles mass transfer model is developed to describe CO2 hydrate crystal thickening at the interface between gas and water. The impacts of gas impurities and channel wettability are also studied. This method is further applied to investigate the conversion of methane hydrate to CO2 hydrate for combined energy recovery and methane hydrate formation. The authors acknowledge the US Department of Energy Basic Energy Science award # DE-SC0022162.
Biological response of eelgrass epifauna, Taylor's Sea hare ( Phyllaplysia taylori ) and eelgrass isopod ( Idotea resecata ), to elevated ocean alkalinity
Abstract. Marine carbon dioxide removal (mCDR) approaches are under development to mitigate the effects of climate change by sequestering carbon in stable reservoirs, with the potential co-benefit of local reductions in coastal acidification impacts. One such method is ocean alkalinity enhancement (OAE). A specific OAE method is the generation of aqueous alkalinity via electrochemistry to enhance the alkalinity of the receiving water by the extraction of acid from seawater, thereby avoiding the issues of solid dissolution kinetics and the release of impurities into the ocean from alkaline minerals. While electrochemical acid extraction is a promising method for increasing the carbon dioxide sequestration potential of the ocean, the biological effects of increasing seawater alkalinity and pH within an OAE project site are relatively unknown. This study aims to address this knowledge gap by testing the effects of increased pH and alkalinity, delivered in the form of aqueous NaOH, on two eelgrass epifauna in the US Pacific Northwest, Taylor's sea hare (Phyllaplysia taylori) and eelgrass isopod (Idotea resecata), chosen for their ecological importance as salmon prey and for their role in eelgrass ecosystems. Four-day experiments were conducted in closed bottles to allow measurements of the evolution of carbonate species throughout the experiment, with water refreshed twice daily to maintain elevated pH, across pHNBS (NBS standard scale) treatments ranging from 7.8 to 9.3. Sea hares experienced mortality in all pH treatments, ranging from 37 % mortality at pHNBS 7.8 to 100 % mortality at pHNBS 9.3. Isopods experienced lower mortality rates in all treatment groups, ranging from 13 % at pHNBS 7.8 to 21 % at pHNBS 9.3, which did not significantly increase with higher pH treatments. These experiments represent an extreme of constant exposure to elevated pH and alkalinity, which should be considered in the context of both the natural variation and the dilution of alkalinity experienced by marine communities across an OAE project site. Different invertebrate species will likely have different responses to increased pH and alkalinity, depending on their physiological vulnerabilities. Investigation of the potential vulnerabilities of local marine species will help inform the decision-making process regarding mCDR planning and permitting.
Computed Tomography Scanning and Petrophysical Measurements of the Wellington KGS 2-32 Core
This report describes the use of the computed tomography facilities and the Multi-Sensor Core Logger at the National Energy Technology Laboratory in Morgantown, West Virginia to characterize core from the Wellington KGS 2-32 well (API 15-191-22770). Core from the well was obtained as part of the Small-Scale Field Test Demonstrating Carbon Dioxide Sequestration in Arbuckle Saline Aquifer and by CO 2 -Enhanced Oil Recovery at Wellington Field, Sumner County, Kansas (DE-FE0006821). The primary impetus of this work was to capture a detailed a digital representation of the core from the Wellington KGS 2-32 well (Sumner County, Kansas). The collaboration between the U.S. Department of Energy’s (DOE) NETL and the Kansas Geological Survey (KGS) at the University of Kansas enables other research entities to access information about this potential carbon storage location and formations. The resultant datasets are presented in this report and can be accessed from NETL's Energy Data eXchange (EDX) online system using the following link: https://edx.netl.doe.gov/dataset/wellington2-32-core.
Assessing Seismic Risk for CO2 Geologic Storage: Comparative Analysis of the Delaware Basin and Basin and Range Province Projects
ABSTRACT: Effective management of induced seismicity is critical for safe and sustainable CO2 storage. This study evaluates fault slippage risks in the Delaware Basin (Texas) and Basin and Range Province (Utah), integrating geological, operational, and geomechanical parameters to assess fault stability and seismic hazard mitigation. In the Delaware Basin, two sites were analyzed under an injection rate of 20,000 bbl/day over 25 years. One site showed low fault slip risk, while the other exhibited higher reactivation potential due to proximity to critically stressed faults. Sensitivity analysis revealed that increased pore pressure significantly heightened slip potential, highlighting the necessity of precise pressure control and real-time monitoring. In the Basin and Range Province, fault stability was evaluated at Neck of the Desert, Escalante Desert, Parowan, and Beaver sites under injection rates of 8,750 bbl/day per site over 30 years. Minimal fault slip risk was observed at Neck of the Desert and Escalante Desert sites, whereas Parowan and Beaver sites exhibited elevated slip potential due to semi-critically stressed faults sensitive to modest pore pressure increases. The findings demonstrate that fault slippage analysis, combined with sensitivity analysis of pore pressure and friction coefficients, is essential for understanding seismic risks. Continuous monitoring, adaptive injection management, and rigorous geomechanical analysis are key strategies for minimizing induced seismicity in CO2 sequestration projects.
Practical Guide to Measuring Wetland Carbon Pools and Fluxes
Abstract Wetlands cover a small portion of the world, but have disproportionate influence on global carbon (C) sequestration, carbon dioxide and methane emissions, and aquatic C fluxes. However, the underlying biogeochemical processes that affect wetland C pools and fluxes are complex and dynamic, making measurements of wetland C challenging. Over decades of research, many observational, experimental, and analytical approaches have been developed to understand and quantify pools and fluxes of wetland C. Sampling approaches range in their representation of wetland C from short to long timeframes and local to landscape spatial scales. This review summarizes common and cutting-edge methodological approaches for quantifying wetland C pools and fluxes. We first define each of the major C pools and fluxes and provide rationale for their importance to wetland C dynamics. For each approach, we clarify what component of wetland C is measured and its spatial and temporal representativeness and constraints. We describe practical considerations for each approach, such as where and when an approach is typically used, who can conduct the measurements (expertise, training requirements), and how approaches are conducted, including considerations on equipment complexity and costs. Finally, we review key covariates and ancillary measurements that enhance the interpretation of findings and facilitate model development. The protocols that we describe to measure soil, water, vegetation, and gases are also relevant for related disciplines such as ecology. Improved quality and consistency of data collection and reporting across studies will help reduce global uncertainties and develop management strategies to use wetlands as nature-based climate solutions.
Deep learning forecasts the spatiotemporal evolution of fluid-induced microearthquakes
Microearthquakes generated by subsurface fluid injection record the evolving stress state and permeability of reservoirs. Forecasting their spatiotemporal evolution is therefore critical for applications such as enhanced geothermal systems, carbon dioxide sequestration and other geoengineering applications. Here we propose a transformer neural network model that ingests hydraulic stimulation history and prior microearthquake observations to forecast four key quantities: cumulative microearthquake count, cumulative logarithmic seismic moment, and the 50th- and 95th-percentile extents of the microearthquake cloud. Applied to the EGS Collab Experiment 1 dataset, the model achieves R2 > 0.98 for the 1-s forecast horizon and R2 > 0.88 for the 15-s forecast horizon across all targets, and supplies uncertainty estimates through a learned standard deviation term. These accurate, uncertainty-quantified forecasts enable real-time inference of fracture propagation and permeability evolution, demonstrating the strong potential of deep-learning approaches to improve seismic-risk assessment and guide mitigation strategies in future fluid-injection operations.
Evolution of Pore Structure and Permeability of Rocks Under Hydrothermal Conditions (Final Report)
The physical and transport properties of porous rocks can be altered by a variety of diagenetic, metamorphic, and tectonic processes, and the changes that result are of critical importance to such industrial applications as resource recovery, carbon dioxide sequestration, and waste isolation in geologic formations. The associated interrelationships between rocks, pore fluids and deformation are also key to understanding many natural processes, including dynamic metamorphism, fault mechanics, fault stability and pressure solution creep. In this project, we investigated the changes of permeability and pore geometry owing to inelastic deformation by solution-transfer, brittle fracturing and dislocation creep. In particular, we studied the coupling between pore fluids and deformation in fluid-filled quartz, calcite, mudstones and ultramafic rocks and examine the effects of coupled mechanical and chemical processes on the evolution of porosity and permeability under hydrothermal conditions. The investigations used a combination of techniques, that included triaxial laboratory experiments; uniaxial compressive loading with in situ observations of microstructure; permeability under hydrostatic compression; observations of microstructure using optical and electron microscopes, and micro-CT imaging; and numerical calculations. Laboratory experiments were designed to provide mechanical and transport data under conditions that isolate the particular mechanisms responsible for the changes. The data obtained were used to quantify changes in surface roughness, porosity, pore dimensions and their spatial fluctuations. The results of the experiments and data from image analyses were compared to the results of network, finite-difference and other numerical models to verify the validity of experimentally established relations between permeability and other rock properties. A bibliography for the period from 2015-2019 is appended below. New results obtained in the final year and the unfunded extension period are detailed below.
Pore architecture controls on mineral reactivity
Mineral dissolution rates measured in natural environments are much slower than those measured in laboratory settings. This project tested the hypothesis that the way fluid flows through rocks in natural systems creates areas where mineral dissolution is fast and areas where mineral dissolution is slow. This hypothesis was tested with a combination of laboratory experiments and numerical simulation. We demonstrated a separation of fluid flow pathways and rates of mineral dissolution in laboratory experiments for the first time using an experimental approach where we created synthetic rocks that have different ratios of connected and dead-end pathways for fluid flow. In laboratory experiments with higher proportions of dead-end pathways, the mineral dissolution rates were slower. We found that where fluid flows through connected pathways the continuous refreshing of fluid at the mineral surface creates conditions where dissolution is fast. In contrast, where fluid either flows slowly through poorly connected pathways or is stagnant in dead-end pathways, mineral dissolution is slow. The results from this project suggest that the overall slowing of rates of mineral dissolution is important when the proportion of dead-end pathways is greater than ~40%. This project informs our understanding of the way that fluids react with rocks in carbon dioxide sequestration and enhanced geothermal projects where fluids are purposefully injected into rocks for energy applications.
Subtask 1.3 – Integrated Carbon Capture and Storage for North Dakota Ethanol Production
The Energy & Environmental Research Center (EERC), in partnership with Red Trail Energy, LLC (RTE), a North Dakota ethanol producer; the North Dakota Industrial Commission (NDIC) Renewable Energy Program (REP); and the U.S. Department of Energy (DOE), conducted a feasibility and implementation study for a commercial carbon capture and storage (CCS) effort. This subtask provided technical support and developed recommended practices of how small-scale industrial CO2 emitters (<1,000,000 tonnes of CO2 emitted annually) may economically deploy CCS. The 64-million-gallon dry mill RTE ethanol facility, emitting an average 180,000 tonnes of CO2 annually, was the subject of the case study. The positive outcome of this research, which shows technical and economic potential for ethanol–CCS in North Dakota, has resulted in RTE acquiring an approved Permit to Drill on December 2, 2019, for a stratigraphic test well in early 2020, a necessary step toward a North Dakota CO2 Storage Facility Permit (SFP) for the RTE CCS effort. Outcomes include 1) validating the Broom Creek Formation as a regional target for CCS, 2) determining the full carbon life cycle of an industrial fuel production facility with CCS, 3) developing a field implementation plan (FIP) for small-scale CCS, and 4) determining the validity and pathway for using CCS to meet low-carbon fuel (LCF) standards. The technical team included the EERC, RTE, Trimeric Corporation, Schlumberger Carbon Services, and Computer Modelling Group (CMG). Findings from activities conducted November 2016 – May 2020 are summarized as follows. Several key steps have been accomplished toward validating the Broom Creek Formation as a CO2 injection and storage target at the RTE CCS site, including verification of the presence and structure of sandstone layers that may comprise the potential CO2 storage reservoir and the several thousand feet of overlying confining zone. Work included site characterization using existing data, interpretation of seismic data within the study area, and geologic modeling simulation of CO2 injection. Interpreted results estimate 3000 feet of confining zone between the Broom Creek Formation (storage target) and the lowermost underground source of drinking water (e.g., the Fox Hills Formation). The thickness of the Broom Creek injection target varies 230–420 ft within the survey area. Results were used to inform the location of a stratigraphic test well and associated characterization test program. No impediments were identified within the targeted CO2 storage complex that would prevent the project from moving forward. A stratigraphic test well is the next step to validate these results and to acquire remaining data necessary to develop a North Dakota CO2 SFP application. The EERC generated full carbon life cycle estimates for CCS integration with the RTE ethanol facility. Results indicated that an average 40% reduction in CO2 emissions is possible through CCS implementation. Approximately half of the carbon in the overall life cycle for a dry mill ethanol plant is generated through the fermentation process and emitted to the atmosphere; this is the CO2 stream targeted for CCS. The remaining carbon is attributed to corn feedstock farming (diesel, fertilizer), energy for fuel processing (natural gas, electricity), and transportation (diesel) of the fuel product. Life cycle carbon estimates are also affected by the anticipated energy consumption of a potential capture facility, which depend on the type of CO2 product generated. For example, a 30%–40% net CO2 emission reduction is estimated if a liquefied CO2 facility were incorporated compared to a 40%–50% net CO2 reduction if a supercritical “injection-grade” CO2 product is generated; i.e., more energy is required to further refine the CO2 stream, affecting the full carbon life cycle estimates. A CCS FIP was developed and initiated at the RTE CCS site, resulting in the development of several guidance documents: a CO2 Capture Process Design Package, a North Dakota CO2 geologic Storage Permits Template, and a Public Outreach Package for CCS in North Dakota. General FIP components include CO2 capture system, pipeline and well designs; monitoring, verification, and accounting (MVA) plans; geologic characterization and testing programs; and permitting and outreach plans. Vendor bids were also acquired for the CO2 liquefaction facility. Near-surface characterization (groundwater and soil gas sampling) and geologic characterization (seismic survey) were initiated to inform development of a UIC Class VI-compliant MVA plan compliant with a North Dakota CO2 SFP. Designs (well and geologic testing) were completed for a stratigraphic test well compliant with a North Dakota CO2 SFP. In addition, the outreach plan was executed, including community open houses, meetings with city/county/state officials, and development of public materials. Although other entities continued to mature incentive programs in 2019–2020, California and the Internal Revenue Service (IRS) currently provide the most advanced economic opportunities for CCS integrated with fuel production. The California Low-Carbon Fuel Standard (LCFS) adopted a CCS Protocol in January 2019, allowing submittal of a design-based pathway (DBP) application for an approved temporary (not certified) carbon intensity value for a fully engineered facility. An ethanol–CCS DBP application to the California LCFS Program (officially approved February 28, 2020) was developed to show that the RTE CCS effort meets LCFS requirements. The approved DBP provides confidence to advance the project and supports potential investments. Other entities continue to mature incentive programs. The IRS issued guidance in February 2020 that addresses the definition of beginning of construction and revenue procedure on partnerships for the Enhancement of Carbon Dioxide Sequestration Credit (a.k.a. Section 45Q) CCS tax credit program; the IRS anticipates issuing further guidance on issues such as secure geologic storage, utilization qualifications, and recapture of claimed credits. Maturing incentive programs coupled with workable permitting regulations provide confidence to advance CCS projects in North Dakota and support financial investment to proceed with designing, constructing, and implementing CCS projects at small-scale fuel production facilities. The largest hurdles for CCS implementation at small-scale industrial systems are often business/economic-related (i.e., not technical). Market uncertainty already exists for agriculture-based alternative fuels such as corn ethanol, for which production has increased by ~33%, and prices have correspondingly lowered since 2015. Passing the Section 45Q tax credit program improves economic feasibility for CCS but may require external investors for a small business to achieve maximum benefits. Public–private partnerships with NDIC and DOE have resulted in foundational technical and regulatory knowledge, growing stakeholder confidence, and a pathway to implementation that enables similar industrial CCS projects in the region to advance. This subtask was funded through the EERC–DOE Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by NDIC and RTE. The authors would also like to thank CMG, ESRI, IHS, Neuralog, and Schlumberger for allowing the use of their software packages in support of this work.
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.
Impacts of Different Operation Conditions and Geological Formation Characteristics on CO2 Sequestration in Citronelle Dome, Alabama
Major concerns of carbon dioxide (CO2) sequestration in subsurface formations are knowledge of the well injectivity and gas storage capacity of the formation, the CO2 pressure and saturation plume extensions during and after injection, and the risks associated with CO2 leakage and fault reactivation. Saline reservoirs are considered as one of the target formations for CO2 sequestration through structural, residual, dissolution, and mineral trapping mechanisms. The boundary condition of the saline reservoir dictates the pressure and saturation plume extension of the injected supercritical CO2 that could expand over large distances. This can lead to sources of risk, e.g., leakage and/or fault reactivation due to presence of wells, thief zones, and geological discontinuities. Therefore, there is a critical need to develop a model that describes how risk-related performance metrics (i.e., the CO2 saturation plume size, the pressure differential plume area, and the pressure differential at specific locations) vary as a function of the size of injection, time following injection, injection operations, and geologic environment. In this study, a systematic reservoir modeling studies of anthropogenic CO2 sequestration in Citronelle dome, Alabama, was performed where all relevant scenarios and conditions to address the questions of the saturation and pressure plume size in the area of review (AoR) and post-injection site care (PISC) are considered. The objective for this study was firstly to systematically simulate CO2 sequestration, i.e., saturation dynamics, and pressure behavior over a range of operational and geological conditions and to derive conclusions about the factors influencing saturation and pressure plume size, post-injection behavior, and the risk associated with them, by developing third-generation reduced order models (ROMs) for reservoir behavior. Finally, to assess the uncertainty associated with our studies, Latin Hypercube Sampling (LHS) together with an experimental design technique, i.e., Plackett–Burman design, was used. Application of Pareto charts and respond surfaces enabled us to determine the most important parameters impacting saturation and pressure plume sizes and to quantify the auto- and cross-correlation among different parameters in both history-matched and upscaled models.