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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Life Cycle Greenhouse Gas Emissions of Growing Intermediate Winter Oilseed Feedstocks for Sustainable Aviation Fuel Production

Ensuring an adequate supply of feedstock is a key challenge to achieving a significant production volume of sustainable aviation fuels (SAFs). One promising feedstock for SAFs is intermediate winter oilseeds added to existing crop production as alternatives to the winter fallow period. In this work, three intermediate winter oilseed crops─camelina ( Camelina sativa L. Crantz .), carinata ( Brassica carinata ), and pennycress ( Thlaspi arvense L .)─are evaluated for their life cycle greenhouse gas (GHG) emissions when harvested and processed into hydroprocessed renewable jet (HRJ). We evaluate solvent extraction (SE) and mechanical pressing as alternative oil extraction methods and examine the impacts of various allocation methods used in the oil extraction process. The GHG emissions reduction potential of camelina-, carinata-, and pennycress-derived HRJs are 50.4%, 65.2%, and 65.7%, respectively, compared to petroleum jet fuel, with SE as an oil extraction method and under mass-based allocation. Combined with the estimated production potential of camelina, carinata, and pennycress as intermediate winter oilseed, 2.5 billion gallons of HRJ can be produced annually, and the total GHG savings could amount to 19.3 million tons when these HRJs replace petroleum jet fuels. In addition, we collect literature information to assess the impacts of these intermediate winter oilseeds on indirect land use change emissions and soil organic carbon sequestration potentials.

camelina↗
DOE OSTI2020

Actinide Separation Inspired by Self-Assembled Metal–Polyphenolic Nanocages

The separation of actinides has a vital place in nuclear fuel reprocessing, recovery of radionuclides, and remediation of environmental contamination. Here we propose a new paradigm of nanocluster-based actinide separation, namely, nanoextraction, that can achieve efficient sequestration of uranium in an unprecedented form of giant coordination nanocages using a cone-shaped macrocyclic pyrogallol[4]arene as the extractant. The U 24 -based hexameric pyrogallol[4]arene nanocages with distinctive [U 2 (PG) 2 ] binuclear units (PG = pyrogallol) that rapidly assembled in situ in monophasic solvent were identified by single-crystal X-ray diffraction, MALDI-TOF mass spectrometry, NMR spectroscopy, and small-angle X-ray and neutron scattering. Furthermore, comprehensive biphasic extraction studies showed that this novel separation strategy has enticing advantages such as fast kinetics, high efficiency, and good selectivity over lanthanides, thereby demonstrating its potential for efficient separation of actinide ions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Controlled Single-Electron Transfer via Metal–Ligand Cooperativity Drives Divergent Nickel-Electrocatalyzed Radical Pathways

Electrocatalysis enables the construction of C-C bonds under mild conditions via controlled formation of carbon-centered radicals. For sequences initiated by alkyl halide reduction, coordinatively unsaturated Ni complexes commonly serve as single-electron transfer agents, giving rise to the foundational question of whether outer- or inner-sphere electron transfer oxidative addition prevails in redox mediation. Indeed, rational design of electrochemical processes requires the discrimination of these two electron transfer pathways, as they can have outsized effects on the rate of substrate bond activation and thus impact radical generation rates and downstream product selectivities. We present results from combined synthetic, electroanalytical, and computational studies that examine the mechanistic differences of single electron transfer to alkyl halides imparted by Ni metal-ligand cooperativity. Electrogenerated reduced Ni species, stabilized by delocalized spin density onto a redox-active tpyPY2Me polypyridyl ligand, activates alkyl iodides via outer-sphere electron transfer, allowing for the selective activation of alkyl iodide substrates over halogen atom donors and the controlled generation and sequestration of electrogenerated radicals. In contrast, the Ni complex possessing a redox-innocent pentapyridine congener activates the substrates in an inner-sphere fashion owning to a purely metal-localized spin, thereby activating both substrates and halogen atom donors in an indiscriminate fashion, generating a high concentration of radicals and leading to unproductive dimerization. Overall, our data establish that controlled electron transfer via Ni-ligand cooperativity can be used to limit undesired radical recombination products and promote selective radical processes in electrochemical environments, providing a generalizable framework for designing redox mediators with distinct rate and potential requirements.

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

Probing pH-Dependent Dehydration Dynamics of Mg and Ca Cations in Aqueous Solutions with Multi-Level Quantum Mechanics/Molecular Dynamics Simulations

The dehydration of aqueous calcium and magnesium cations is the most fundamental process controlling their reactivity in chemical and biological phenomena, such as the formation of ionic solids or passing through ion channels. It holds particular relevance in light of recent advancements in the development of carbon capture techniques that rely on mineralization for long-term carbon storage. Specifically, dehydration of Ca 2+ and Mg 2+ is a key step in proposed carbon capture processes aiming to exploit the relatively high concentration of dissolved carbon dioxide in seawater via the formation of carbonate minerals from solvated Ca 2+ and Mg 2+ cations for sequestration and storage. Nevertheless, atomic-scale understanding of the dehydration of aqueous Ca 2+ and Mg 2+ cations remains limited. Here, we utilize rare event sampling via density functional theory molecular dynamics and embedded wavefunction theory calculations to elucidate the dehydration dynamics of aqueous Ca 2+ and Mg 2+ . Emphasis is placed on the investigation of the effect pH has on the stability of the different coordination environments. Here, our results reveal significant differences in the dehydration dynamics of the two cations and provide insight into how they may be modulated by pH changes.

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

Tailoring Hierarchical Structure and Rare Earth Affinity of Compositionally Identical Polymers via Sequence Control

Macromolecule sequence, structure, and function are inherently intertwined. While well-established relationships exist in proteins, they are more challenging to define for synthetic polymer nanoparticles due to their molecular weight, sequence, and conformational dispersities. Furthermore, to explore the impact of sequence on nanoparticle structure, we synthesized a set of 16 compositionally identical, sequence-controlled polymers with distinct monomer patterning of dimethyl acrylamide and a bioinspired, structure-driving di(phenylalanine) acrylamide (FF). Sequence control was achieved through multiblock polymerizations, yielding unique ensembles of polymer sequences which were simulated by kinetic Monte Carlo simulations. Systematic analysis of the global (tertiary- and quaternary-like) structure in this amphiphilic copolymer series revealed the effect of multiple sequence descriptors: the number of domains, the hydropathy of terminal domains, and the patchiness (density) of FF within a domain, each of which impacted both chain collapse and the distribution of single- and multichain assemblies. Furthermore, both the conformational freedom of chain segments and local-scale, β-sheet-like interactions were sensitive to the patchiness of FF. To connect sequence, structure, and target function, we evaluated an additional series of nine sequence-controlled copolymers as sequestrants for rare earth elements (REEs) by incorporating a functional acrylic acid monomer into select polymer scaffolds. We identified key sequence variables that influence the binding affinity, capacity, and selectivity of the polymers for REEs. Collectively, these results highlight the potential of and boundaries of sequence control via multiblock polymerizations to drive primary sequence ensembles hierarchical structures, and ultimately the functionality of compositionally identical polymeric materials.

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

Enriched Molecular-Level View of Saline Wetland Soil Carbon by Sensitivity-Enhanced Solid-State NMR

Soil organic matter (SOM) plays a major role in mitigating greenhouse gas emission and regulating earth’s climate, carbon cycle, and biodiversity. Wetland soils account for one-third of all SOM; however, globally, coastal wetland soils are eroding faster due to increasing sea-level rise. Our understanding of carbon sequestration dynamics in wetlands lags behind that of upland soils. Here, we employ solid-state nuclear magnetic resonance (ssNMR) to investigate the molecular-level structure of biopolymers in wetland soils spanning 11 centuries. High-resolution multidimensional spectra, enabled by dynamic nuclear polarization (DNP), demonstrate enduring preservation of molecular structures within herbaceous plant cores, notably condensing aromatic motifs and carbohydrates, even over a millennium, with the preserved cores constituting a decreasing minority among molecules from decomposition and repolymerization with depth and age. Such preserved cores occur alongside molecules from the decomposition of loosely packed parent biopolymers. These findings emphasize the relative vulnerability of coastal wetland SOM when exposed to oxygenated water due to geological and anthropogenic changes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Rapid Mineral Precipitation During Shear Fracturing of Carbonate-Rich Shales

Target subsurface reservoirs for emerging low-carbon energy technologies and geologic carbon sequestration typically have low permeability and thus rely heavily on fluid transport through natural and induced fracture networks. Sustainable development of these systems requires deeper understanding of how geochemically mediated deformation impacts fracture microstructure and permeability evolution, particularly with respect to geochemical reactions between pore fluids and the host rock. Here, a series of triaxial direct shear experiments was designed to evaluate how fractures generated at subsurface conditions respond to penetration of reactive fluids with a focus on the role of mineral precipitation. Calcite-rich shale cores were directly sheared under 3.5 MPa confining pressure using BaCl 2 -rich solutions as a working fluid. Experiments were conducted within an X-ray computed tomography (xCT) scanner to capture 4-D evolution of fracture geometry and precipitate growth. Three shear tests evidenced nonuniform precipitation of barium carbonates (BaCO 3 ) along through-going fractures, where the extent of precipitation increased with increasing calcite content. Precipitates were strongly localized within fracture networks due to mineral, geochemical, and structural heterogeneities and generally concentrated in smaller apertures where rock:water ratios were highest. The combination of elevated fluid saturation and reactive surface area created in freshly activated fractures drove near-immediate mineral precipitation that led to an 80% permeability reduction and significant flow obstruction in the most reactive core. While most previous studies have focused on mixing-induced precipitation, this work demonstrates that fluid–rock interactions can trigger precipitation-induced permeability alterations that can initiate or mitigate risks associated with subsurface energy systems.

58 GEOSCIENCES↗
DOE OSTI2020

Distributed Acoustic Sensing as a Distributed Hydraulic Sensor in Fractured Bedrock

Distributed acoustic sensing (DAS) was originally intended to measure oscillatory strain at frequencies of 1 Hz or more on a fiber optic cable. Recently, measurements at much lower frequencies have opened the possibility of using DAS as a dynamic strain sensor in boreholes. A fiber optic cable mechanically coupled to a geologic formation will strain in response to hydraulic stresses in pores and fractures. A DAS interrogator can measure dynamic strain in the borehole, which can be related to fluid pressure through the mechanical compliance properties of the formation. Because DAS makes distributed measurements, it is capable of both locating hydraulically active features and quantifying the fluid pressure in the formation. We present field experiments in which a fiber optic cable was mechanically coupled to two crystalline rock boreholes. The formation was stressed hydraulically at another well using alternating injection and pumping. The DAS instrument measured oscillating strain at the location of a fracture zone known to be hydraulically active. Rock displacements of less than 1 nm were measured. Laboratory experiments confirm that displacement is measured correctly. These results suggest that fiber optic cable embedded in geologic formations may be used to map hydraulic connections in three-dimensional fracture networks. A great advantage of this approach is that strain, an indirect measure of hydraulic stress, can be measured without beforehand knowledge of flowing fractures that intersect boreholes. The technology has obvious applications in water resources, geothermal energy, CO 2 sequestration, and remediation of groundwater in fractured bedrock.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Contrasting Responses of Soil Inorganic Carbon to Afforestation in Acidic Versus Alkaline Soils

Afforestation is recommended as an effective approach for carbon sequestration and environmental benefits. However, it remains less clear, and sometimes controversial, regarding how afforestation may impact soil inorganic carbon (SIC), a crucial component of the ecosystem carbon pool. Here, using field data from 619 afforested plots and 163 control plots across northern China, we investigated the relative and absolute differences in SIC between afforested and corresponding control plots. Our results suggested that afforestation increased SIC in acidic soils, while decreased SIC in alkaline soils. Fitting a linear mixed model and further a structure equation model, we found that afforestation-induced soil pH change was the most significant factor regulating SIC responses. In particular, SIC was more sensitive to pH change in more arid areas, where both soil pH and SIC stocks were high. Other factors could indirectly affect SIC responses to afforestation through modulating soil pH and soil organic carbon (SOC) dynamics. Moreover, afforestation-induced SIC changes also varied considerably among different species of tree plantations and across different soil depths. Importantly, in plantations of Pinus sylvestris var. mongholica, Pinus tabuliformis, and Populus spp., changes in SIC caused by afforestation were even comparable to that in SOC. Overall, our findings provide a data-based understanding on the comprehensive soil carbon dynamics following afforestation and its underlying mechanisms. With the increased use of afforestation and reforestation as nature-based solutions to climate change, their associated impacts on SIC need to be taken into account, especially in SIC-rich areas.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

From Fluid Flow to Coupled Processes in Fractured Rock: Recent Advances and New Frontiers

Abstract Quantitative predictions of natural and induced phenomena in fractured rock is one of the great challenges in the Earth and Energy Sciences with far‐reaching economic and environmental impacts. Fractures occupy a very small volume of a subsurface formation but often dominate fluid flow, solute transport and mechanical deformation behavior. They play a central role in CO 2 sequestration, nuclear waste disposal, hydrogen storage, geothermal energy production, nuclear nonproliferation, and hydrocarbon extraction. These applications require predictions of fracture‐dependent quantities of interest such as CO 2 leakage rate, hydrocarbon production, radionuclide plume migration, and seismicity; to be useful, these predictions must account for uncertainty inherent in subsurface systems. Here, we review recent advances in fractured rock research covering field‐ and laboratory‐scale experimentation, numerical simulations, and uncertainty quantification. We discuss how these have greatly improved the fundamental understanding of fractures and one's ability to predict flow and transport in fractured systems. Dedicated field sites provide quantitative measurements of fracture flow that can be used to identify dominant coupled processes and to validate models. Laboratory‐scale experiments fill critical knowledge gaps by providing direct observations and measurements of fracture geometry and flow under controlled conditions that cannot be obtained in the field. Physics‐based simulation of flow and transport provide a bridge in understanding between controlled simple laboratory experiments and the massively complex field‐scale fracture systems. Finally, we review the use of machine learning‐based emulators to rapidly investigate different fracture property scenarios and accelerate physics‐based models by orders of magnitude to enable uncertainty quantification and near real‐time analysis.

58 GEOSCIENCES↗
DOE OSTI2021

Diffusion-to-Imbibition Transition in Water Sorption in Nanoporous Media: Theoretical Studies

The ability to predict multiphase fluid transport in nanoporous rocks such as shales is critical for many geoscience applications, for example unconventional hydrocarbon production, geologic carbon sequestration, and nuclear waste disposal. When the pore sizes approach nanoscales, the impact of the molecular interaction forces between fluids and solids becomes increasingly important. These forces can alter macroscopic fluid phase behavior and control transport. Recent experimental studies have shown that capillary condensation and subsequent imbibition of liquid water can occur in hydrophilic nanoporous media even if the vapor phase is at a critical relative humidity (rhcrit) well below vapor saturation. This study presents a theoretical investigation of the processes controlling adsorption, capillary condensation and imbibition in nanoporous media, using the square-gradient classical density functional theory. The proposed theoretical model explicitly includes the relevant interaction forces among fluids and solids in macroscopic porous media. Application of the model to a relative-humidity-controlled water adsorption experiment is presented to demonstrate the impact of water-pore wall attractive forces on multiphase water behavior in a hydrophilic silicon nanoporous medium. Here, the model represents well the measured time-dependent evolution of the water imbibition front inside the nanoporous medium and also explains the diffusion-like water transport regimes observed at rh < rh crit and the imbibition-like flow regimes observed at rh > rh crit . The study furthermore gives an insight on hysteresis phenomenon in adsorption and desorption isotherms.

58 GEOSCIENCES↗
DOE OSTI2021

Impacts of Pore Network-Scale Wettability Heterogeneity on Immiscible Fluid Displacement: A Micromodel Study

The mixed-wet nature of reservoir formations imposes a wide range of rock wettability from strong resident-fluid wetting to strong invading-fluid wetting. The characteristics of two-phase flow in porous media composed of mixed-wetting surfaces remain poorly understood. In this study, we investigated the displacement of resident ethylene glycol (EG) by hexane in two mixed-wet micromodels of identical 2.5-D geometry heterogeneity, with uniformly or heterogeneously distributed patches strongly wetting to hexane. These patches are mixed among pores with unaltered EG-wetting surfaces. Along with control tests in the originally EG-wet micromodel, here we show the classic fingering and transitions in flow regimes at $logCa$ (capillary number) from -7.2 to -3.9. Moreover, pore-scale distributions of wettability and their spatial correlation influence displacement efficiency. In the two mixed-wet micromodels, we found (a) an increase of steady-state hexane saturation at the end of experiments by up to 0.12 in the capillary fingering regime and a decrease of at most by 0.06 in the viscous fingering regime, compared to the EG-wet micromodel, and (b) dispersed and fragmented hexane distribution after displacement. Brine drainage during supercritical CO 2 (scCO 2 ) injections in these micromodels occurs with lower wettability contrasts, and under similar viscosity ratios and interfacial tensions resulted in higher displacement efficiency relative to displacement of EG by hexane. While mixed-wettability can enhance displacement efficiency compared to uniform wettability, the dynamics of immiscible fluids in strong mixed-wet reservoirs are expected to be less pronounced in contributing to the efficiency of geological CO 2 sequestration, oil recovery, and remediation of hydrocarbon-contaminated aquifers.

2.5-D micromodel↗
DOE OSTI2022

Atmospheric Radiative and Oceanic Biological Productivity Responses to Increasing Anthropogenic Combustion‐Iron Emission in the 1850–2010 Period

Abstract Anthropogenic emission is an important component of the present‐day iron cycle yet its long‐term impacts on climate are poorly understood. Iron mineralogy strongly affects its radiative and oceanic interactions and was unrepresented in previous studies. We perform simulations using a mineralogy‐based inventory and an atmospheric transport model and estimate the 1850–2010 global mean direct radiative forcing (DRF) to be +0.02 to +0.10 W/m 2 . We estimate that the CO 2 sequestration of 0.2–13 ppmv over the last 150 years due to enhanced phytoplankton productivity by anthropogenic iron deposition causes an avoided CO 2 forcing of −0.002 to −0.16 W/m 2 . While globally small, these impacts can be higher in specific regions; the anthropogenic DRF is +0.5 W/m 2 over areas with more coal combustion and metal smelting, and anthropogenic soluble iron sustains >10% of marine net primary productivity in the high‐latitude North Pacific Ocean, a region vulnerable to stratification due to climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Reactive Transport Modeling of Mineral Precipitation and Carbon Trapping in Discrete Fracture Networks

In this study we use numerical experiments to analyze reactive flow and transport behavior in discrete intersecting fracture networks, focusing on (a) how reaction-induced changes in physical and chemical properties affect flow connectivity and (b) how fracture networks developed in the Earth's critical zone contribute to carbon sequestration via mineral weathering reactions. In the first part of the study, we used two-dimensional reactive flow and transport simulations to analyze the impacts of mixing in a natural discrete fracture network. We concluded that reaction-induced changes can substantially alter the flow connectivity, especially at fracture intersections. The second set of simulations considered the problem of natural weathering of fractured mafic and ultramafic rocks in the partially saturated Earth's critical zone as a function of infiltration rates, fracture permeability, and partially saturated flow parameters. As a model system, we considered an incongruent reaction network with dissolution of forsterite and precipitation of magnesite. The behavior is complex in terms of the rate-controlling processes because of the multicomponent nature of the system as shown by the grid Peclet number: the CO 2 behavior is gas diffusion-controlled in the partially saturated zone, while the rate of water flow via the Damkӧhler number controls Mg 2+ transport through the fracture network. The amounts of carbon that can be trapped are modest, but the naturally fractured domain considered here provides a useful “base case” against which various engineered solutions can be compared.

58 GEOSCIENCES↗
DOE OSTI2022

Leakage From Coexisting Geologic Forcing and Injection‐Induced Pressurization: A Semi‐Analytical Solution for Multilayered Aquifers With Multiple Wells

Abstract Abnormal fluid pressures (above or below hydrostatic pressure) can develop and persist in sedimentary basins. The common occurrence of abnormal pressures may cause challenges for project permitting of geological carbon sequestration (GCS), particularly in reservoirs with pre‐injection overpressure. The leaky wells that may exist in some sedimentary basins can provide flow paths between deep brine aquifers and shallower freshwater aquifers. Pre‐injection relative overpressures can cause brine leakage through leaky wells even before any injection occurs. The tendency for flow through leaky wells is coupled with the process of pressure dissipation that occurs through aquitards. Specifically, with non‐zero permeability, aquitards can dissipate pressure over large areal extents and thereby reduce leakage rates through leaky wells. This study presents development of a semi‐analytical solution for hydraulic head and brine leakage in multilayered aquifer–aquitard systems with geologic pressure forcing. The geologic forcing that causes abnormal pressures in the multilayered system can coexist with any number of injection, extraction, and leaky wells that also affect fluid pressure. The semi‐analytical model is applied to explore how leakage through leaky wells varies as functions of pressurization rate, along with aquitard and leaky well properties in an overpressured multilayered system. The results show that although injection‐induced pressures can dissipate rapidly through suitably permeable aquitards, coexisting geologic forcing may create sustained rates of brine leakage into freshwater aquifers through leaky wells. In GCS, a very low‐permeability aquitard with high capillary entry pressure to free‐phase CO 2 is desired to serve as the caprock to prevent leakage of CO 2 from the storage reservoir. Nevertheless, the results from this study show that the brine leakage impact to shallow freshwater aquifers through leaky wells might substantially decrease with increasing aquitard permeability values, as long as small aquitard permeability and high capillary entry pressure serve to prevent CO 2 leakage.

Cihan, A.↗
DOE OSTI2023

Compost Amendment to a Grazed California Annual Grassland Increases Gross Primary Productivity Due To a Longer Growing Season

Abstract Compost amendment to rangelands is a proposed nature‐based climate solution to increase plant productivity and soil carbon sequestration. However, it has not been evaluated using quasicontinuous ecosystem‐scale measurements. Here, we present the first study to utilize eddy covariance and footprint partitioning to monitor carbon exchange in a grassland with and without compost amendment, monitoring for 1 year before and 1 year after treatment. Compost amendment to an annual California grassland was found to enhance net ecosystem removal of carbon. Our study confirmed that compost‐amended grasslands, similar to nonamended grasslands, are net carbon sources to the atmosphere; however, the amendment appears to be slowing down the rate at which these ecosystems lose carbon by 0.71 Mg C ha −1 per growing season. Digital repeated imagery of the canopy revealed that compost‐amended grasslands experienced an earlier green‐up, resulting in an overall longer growing season by >60 days. Notably, we did not detect significantly higher amounts of soil carbon in compost‐amended soils. High variability in soil carbon demands greater sampling replication in future studies. A longer growing season and higher productivity are hypothesized to be a result of greater availability of macronutrients and micronutrients in the top layer of soil (specifically nitrogen, phosphorus, and zinc).

Fenster, Tommy L. D.↗
DOE OSTI2024

Carbon Mineralization in Fractured Mafic and Ultramafic Rocks: A Review

Mineral carbon storage in mafic and ultramafic rock masses has the potential to be an effective and permanent mechanism to reduce anthropogenic CO 2 . Several successful pilot-scale projects have been carried out in basaltic rock (e.g., CarbFix, Wallula), demonstrating the potential for rapid CO 2 sequestration. However, these tests have been limited to the injection of small quantities of CO 2 . Thus, the longevity and feasibility of long-term, large-scale mineralization operations to store the levels of CO 2 needed to address the present climate crisis is unknown. Moreover, CO 2 mineralization in ultramafic rocks, which tend to be more reactive but less permeable, has not yet been quantified. In these systems, fractures are expected to play a crucial role in the flow and reaction of CO 2 within the rock mass and will influence the CO 2 storage potential of the system. Therefore, consideration of fractures is imperative to the prediction of CO 2 mineralization at a specific storage site. In this review, we highlight key takeaways, successes, and shortcomings of CO 2 mineralization pilot tests that have been completed and are currently underway. Laboratory experiments, directed toward understanding the complex geochemical and geomechanical reactions that occur during CO 2 mineralization in fractures, are also discussed. Experimental studies and their applicability to field sites are limited in time and scale. Many modeling techniques can be applied to bridge these limitations. We highlight current modeling advances and their potential applications for predicting CO 2 mineralization in mafic and ultramafic rocks.

25 ENERGY STORAGE↗
DOE OSTI2023

Emergence of Unstable Focused Flow Induced by Variable‐Density Flows in Vertical Fractures

Abstract Fluids with different densities often coexist in subsurface fractures and lead to variable‐density flows that control subsurface processes such as seawater intrusion, contaminant transport, and geologic carbon sequestration. In nature, fractures have dip angles relative to gravity, and density effects are maximized in vertical fractures. However, most studies on flow and transport through fractures are often limited to horizontal fractures. Here, we study the mixing and transport of variable‐density fluids in vertical fractures by combining three‐dimensional (3D) pore‐scale numerical simulations and visual laboratory experiments. Two miscible fluids with different densities are injected through two inlets at the bottom of a fracture and exit from an outlet at the top of the fracture. Laboratory experiments show the emergence of an unstable focused flow path, which we term a “runlet.” We successfully reproduce the unstable runlet using 3D numerical simulations and elucidate the underlying mechanisms triggering the runlet. Dimensionless number analysis shows that the runlet instability arises due to the Rayleigh‐Taylor instability (RTI), and flow topology analysis is applied to identify 3D vortices that are caused by the RTI. Even under laminar flow regimes, fluid inertia is shown to control the runlet instability by affecting the size and movement of vortices. Finally, we confirm the emergence of a runlet in rough‐walled fractures. Since a runlet dramatically affects fluid distribution, residence time, and mixing, the findings in this study have direct implications for the management of groundwater resources and subsurface applications.

Environmental Sciences & Ecology↗