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DOE OSTI2026

Modeling supercritical CO 2 flow and mineralization in reactive host rocks with PFLOTRAN v7.0

Understanding the flow and reactivity of CO 2 injected into geological reservoirs is important for many subsurface applications including secure geologic carbon storage (GCS), critical mineral extraction, enhanced geothermal systems (EGS), and enhanced oil recovery (EOR). Traditionally, subsurface CO 2 injection for GCS applications has focused on geologic formations with favorable subsurface configurations for CO 2 migration and trapping through non-reactive mechanisms such as structural, solubility, and petrophysical trapping. Recently, CO 2 -reactive rocks such as mafic and ultramafic basalts have been investigated for their potential to react with injected CO 2 in situ to simultaneously dissolve host rock minerals and mineralize CO 2 as carbonates. Engineering rapid CO 2 mineralization in the subsurface is attractive because of the increased density of stored CO 2 , the additional safety factors associated with solidification, and the potential to extract valuable critical minerals. Here we present recent developments in the parallel flow and reactive transport simulator PFLOTRAN to model coupled CO 2 -brine flow and reactive transport for a wide range of injection and production applications involving reactive CO 2 -brine systems. These developments are based on the well established and trusted CO 2 flow capabilities in the STOMP-CO 2 simulator. New capabilities added to PFLOTRAN include new CO 2 -brine equations of state with optional thermal coupling, several new constitutive relationships like capillary pressure smoothing and scanning path hysteresis, a fully implicit well model, and native linkage with PFLOTRAN's well-established reactive transport libraries. A series of benchmarks between PFLOTRAN and STOMP-CO 2 verify the newly developed CO 2 -brine flow capabilities. Demonstrations of coupled CO 2 -brine flow modeling and reactive transport show how CO 2 mineralization can be engineered in reactive host rocks. Finally, an example use case involving copper leaching by CO 2 and critical mineral extraction is presented to showcase the strengths of this new implementation. Several limitations still remain, including limited availability of field data to parameterize models. Future work should constrain the evolution of mineral surface area during mineralization and the temperature and/or pH dependence of geochemical reactions for specific systems of interest.

Critical Minerals↗

DOE OSTI2021

Spontaneous Imbibition Tests and Parameter Estimation in Volcanic Tuff

We present a dynamic laboratory spontaneous imbibition test and interpretation method, demonstrated on volcanic tuff samples from the Nevada National Security Site. The method includes numerical inverse modeling to quantify uncertainty of estimated two-phase fluid flow properties. As opposed to other approaches requiring multiple different laboratory instruments, the dynamic imbibition method simultaneously estimates capillary pressure and relative permeability from one test apparatus.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Capillary-Enhanced Two-Phase Micro-Cooler Using Copper-Inverse-Opal Wick with Silicon Microchannel Manifold for High-Heat-Flux Cooling Application

In this work, we demonstrate a two-phase capillary-fed boiling micro-cooler that consists of a ~ 25-..mu..m-thick copper inverse opal (CIO) porous wicking structure for high-heat-flux boiling and a silicon 3D-manifold for distributed liquid delivery and vapor extraction across a 0.5 cm x 0.5 cm heated area. At low inlet water mass flow rates of 1.5 to 1.9 g(min)-1, the micro-cooler displays nearly two-phase boiling with exit vapor quality ~ 1 and a high critical heat flux (CHF) of 253 to 320 W cm-2 with low superheat of ~ 10 degrees C resulting in a thermal resistance of boiling ~ 0.025 cm2 degrees C W-1 or heat transfer coefficient of 0.4 MW m-2 degrees C-1. For higher flow rates of 5, 10, and 15 g(min)-1, the micro-cooler exhibits a hybrid single-phase and two-phase cooling regime where the contribution of the sensible heat (single-phase) cooling is linearly added to that of the two-phase cooling. For the highest flow rate of 15 g(min)-1, the CHF is increased to ~ 500 W cm-2 resulting in an overall thermal resistance of ~ 0.18 cm2 degrees C W-1. However, the two-phase heat transfer effectiveness, which estimates the utilization level of the inlet mass flow rate for two-phase boiling, is reduced to ~ 0.11. To achieve the best cooling system performances, the micro-cooler must operate entirely within the two-phase boiling regime (exit vapor quality or two-phase heat transfer effectiveness ~ 1). Ideally, the "coolant" should be delivered near its saturation temperature (~ 100 degrees C for water), which provides significant advantages for the energy-efficient operation of data centers and power electronics. We present detailed analysis with Infrared and high speed camera images at various inlet flow rates and heat fluxes to understand complex heat transfer in the micro-cooler. Furthermore, a conjugate thermofluidic simulation model, which incorporates the physics of capillary-fed boiling in a porous copper layer, agrees well with the experimental data.

capillary-enhanced boiling↗

DOE OSTI2025

SPE-CZE-MS Quantifies Zeptomole Amounts of Phosphorylated Peptides

Capillary zone electrophoresis (CZE) is gaining attention in the field of single-cell proteomics for its ultralow-flow and high-resolution separation abilities. Even more sample-limited yet rich in biological information are phosphoproteomics experiments, as the phosphoproteome composes only a fraction of the whole cellular proteome. Rapid analysis, high sensitivity, and maximization of sample utilization are paramount for single-cell analysis. Some challenges of coupling CZE analysis with mass spectrometry analysis (MS) of complex mixtures include 1. sensitivity due to volume loading limitations of CZE and 2. incompatibility of MS duty cycles with electropherographic time scales. Here, we address these two challenges as applied to singlecell- equivalent phosphoproteomics experiments by interfacing a microchip-based CZE device integrated with a solid-phaseextraction (SPE) bed with the Orbitrap Astral mass spectrometer. Using 225 phosphorylated peptide standards and phosphorylated peptide-enriched mouse brain tissue, we investigate microchip-based SPE-CZE functionality, quantitative performance, and complementarity to nano-LC-MS (nLC-MS) analysis. We highlight unique SPE-CZE separation mechanisms that can empower fitfor- purpose applications in single-cell-equivalent phosphoproteomics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Integrated Molten Salt Reactor Modeling Capabilities in NEAMS Thermal Hydraulics Tools

The DOE neams program supports a full range of computational thermal fluids analysis capabilities and code developments for a broad range of advanced reactor concepts. The research and development approach under the thermal fluids technical area synergistically combines three length and time scales in a hierarchical multi-scale approach. To enable multi-scale thermal fluids capability using these codes, a key joint effort has been underway to develop an integrated system- and engineering-scale thermal fluids analysis capability, through integration of SAM and Pronghorn codes, both based on the MOOSE framework. This report summarizes recent advances in developing an integrated system- and engineering-scale modeling capability for the msr concept, which has gained significant interest in recent years. A consistent framework was established by coupling Pronghorn and SAM through the Saline interface, with thermophysical properties provided by the Molten Salt Thermal Property Database (MSTDB-TP). Further improvements were made to the coupling schemes and domain-overlapping strategies, enhancing the stability and robustness of multi-code simulations. Verification and validation efforts demonstrate the accuracy of this integration across a range of benchmark problems, including one-dimensional heated pipe flows, three-dimensional natural convection loops with evolving isotopic compositions, and \gls{msre} demonstration cases. Within Pronghorn, new capabilities were introduced to model corrosion and noble-metal plating phenomena, supported by an extended thermal-hydraulics framework and refined turbulence treatments. To capture two-phase flow behavior, a multiphase Euler–Euler model was implemented in Pronghorn, including advanced closure relations, high-resolution advection techniques, and capillary force reconstruction. Preliminary verification cases confirm the fidelity of the approach, while planned validation efforts target canonical multiphase benchmarks and application to msr components such as the msre pump bowl. Finally, updates to SAM’s msr mass transfer modeling were extended to consider noble gas migration into porous structures like graphite. The point kinetics model was updated to include reactivity feedback contributions from any defined species, such as xenon. The gas transport model was expanded for applicability to gas mixtures, bubble efflux phenomena, and species transport between liquid and gas phases. A selection of multi-scale Sherwood number correlations from MOSCATO/NekRS and multi-phase correlations from literature have been added for improved accuracy in calculating mass transfer coefficients. A companion effort on developing system-level redox corrosion has also been incorporated into SAM. Collectively, these enhancements strengthen the predictive capability of SAM and Pronghorn for simulating MSR thermal-hydraulics, corrosion, multiphase behavior, and fission-product transport, providing a more complete toolset for design, safety analysis, and licensing support of next-generation \gls{msr}s.

42 - ENGINEERING↗

DOE OSTI2021

Towards replacing physical testing of granular materials with a Topology-based Model

In the study of packed granular materials, the performance of a sample (e.g., the detonation of a high-energy explosive) often correlates to measurements of a fluid flowing through it. The “effective surface area,” the surface area accessible to the airflow, is typically measured using a permeametry apparatus that relates the flow conductance to the permeable surface area via the Carman-Kozeny equation. This equation allows calculating the flow rate of a fluid flowing through the granules packed in the sample for a given pressure drop. However, Carman-Kozeny makes inherent assumptions about tunnel shapes and flow paths that may not accurately hold in situations where the particles possess a wide distribution in shapes, sizes, and aspect ratios, as is true with many powdered systems of technological and commercial interest. To address this challenge, we replicate these measurements virtually on micro-CT images of the powdered material, introducing a new Pore Network Model based on the skeleton of the Morse-Smale complex. Pores are identified as basins of the complex, their incidence encodes adjacency, and the conductivity of the capillary between them is computed from the cross-section at their interface. We build and solve a resistive network to compute an approximate laminar fluid flow through the pore structure. Here, we provide two means of estimating flow-permeable surface area: (i) by direct computation of conductivity, and (ii) by identifying dead-ends in the flow coupled with isosurface extraction and the application of the Carman-Kozeny equation, with the aim of establishing consistency over a range of particle shapes, sizes, porosity levels, and void distribution patterns.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Counter gravity heat pipe techniques

A pump assisted heat pipe may combine the low mass flow rate required of latent heat pipe transfer loops with a hermetically sealed pump to overcome the typical heat pipe capillary limit. This may result in a device with substantially higher heat transfer capacity over conventional pumped single-phase loops, heat pipes, loop heat pipes, and capillary pumped loops with very modest power requirements to operate. Further, one or more embodiments overcome the gravitation limitations in the conventional heat pipe configuration, e.g., when the heat addition zone is above the heat rejection zone, the capillary forces are required to transfer the liquid from the heat rejection zone to the heat addition zone against gravity.

Reid, Robert S.↗

DOE OSTI2024

Equivalence Ratio Scans in a Rotating Detonation Engine

Published data for run times exceeding a few seconds in rotating detonation engines (RDEs) is rare, but long duration tests are necessary to understand both transient and persistent phenomena in RDE operation. Previous work has noted different detonation wave modes at different equivalence ratios. In the current study, multiple long-duration runs with constant air flow rate and variable equivalence ratio are conducted in a hydrogen-fueled, water-cooled RDE. Analysis of the capillary tube averaged pressure (CTAP) data reveals a strong correlation with equivalence ratio as well as a small time dependency due to transient thermal processes. Ion probe measurements are used to analyze detonation wave frequencies and modes, both of which are strongly dependent on the equivalence ratio. Mode transitions are observed to occur consistently as the equivalence ratio is traversed between 0.55 and 0.60. These transitions are also found to be a function of the direction of changing equivalence ratio (ascending or descending) and time.

Boyette, Wesley R.↗

DOE OSTI2024

Equivalence Ratio Scans in a Rotating Detonation Engine

Boyette, Wesley R.↗

DOE OSTI2024

Counter gravity heat pipe techniques

Reid, Robert S.↗

DOE OSTI2023

Helium-3 Piping and Gas Handling Implementation for the Colossus milli-Kelvin Platform at Fermilab

Colossus is a large millikelvin platform that has a two-meter diameter mixing chamber plate. This uniquely large millikelvin platform utilizes a cryogenics plant to maintain progressively lower temperatures at each of the three upper stages and precool the lower three stages of the system. At the millikelvin stages, Colossus employs multiple commercially available dilution units to achieve millikelvin temperatures at the 100 mK and 20 mK stages. The incoming helium-3/helum-4 process fluid mixture for each dilution unit flows through tubes wrapped around copper posts attached to each of the upper stages of the system. These tubes function as capillary heat exchanger to reduce the temperature of the incoming helium mixture to the appropriate temperature at each stage.

James, C.↗

DOE OSTI2025

Temporal persistence of postfire flood hazards under present and future climate conditions in southern Arizona, USA

Changes to soil hydraulic properties that reduce infiltration capacity following fire can increase flash flood risks. These risks are exacerbated by rainfall intensification associated with a warming climate. However, the potential effects of climate-change-driven rainfall intensification on postfire floods remain largely unexplored. Using rainfall and runoff observations from a 49.4 km 2 watershed in southern Arizona, USA, and a hydrologic model (KINEROS2), we examined the temporal evolution following a historic fire of three crucial hydrologic parameters: soil saturated hydraulic conductivity (K sp ), net capillary drive (G p ), and hydraulic roughness (n c ). We explored how the effect of fire on these parameters may influence peak flow under future climate scenarios derived from CMIP6, specifically the medium emissions scenario (SSP2-4.5) and high emissions scenario (SSP5-8.5). Results demonstrate an increase in K sp from 11 mm h −1 in the first postfire year to 60 mm h −1 in postfire year 3. G p similarly increased from 19 mm in the first postfire year to 30 mm in the third, while nc was relatively constant. The highest simulated Q p occurred in the first postfire year. Under the SSP2-4.5 scenario, the likelihood of a 100-year flood is projected to be twice as large by the middle of the century relative to its historical magnitude. Simulations further indicate that the maximum expected discharge associated with a postfire flood, as derived from historical data, could be triggered by a 10-year rainstorm under the SSP5-8.5 scenario by the late century. Simulations also demonstrate that rainfall intensification will lead to greater persistence of elevated flood hazards following fire by the late century under both the SSP2-4.5 and the SSP5-8.5 scenarios.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Two-Phase Flow Mechanisms Controlling CO2 Intrusion into Shaly Caprock

Abstract Geologic carbon storage in deep saline aquifers has emerged as a promising technique to mitigate climate change. CO 2 is buoyant at the storage conditions and tends to float over the resident brine jeopardizing long-term containment goals. Therefore, the caprock sealing capacity is of great importance and requires detailed assessment. We perform supercritical CO 2 injection experiments on shaly caprock samples (intact caprock and fault zone) under representative subsurface conditions. We numerically simulate the experiments, satisfactorily reproducing the observed evolution trends. Simulation results highlight the dynamics of CO 2 flow through the specimens with implications to CO 2 leakage risk assessment in field practices. The large injection-induced overpressure drives CO 2 in free phase into the caprock specimens. However, the relative permeability increase following the drainage path is insufficient to provoke an effective advancement of the free-phase CO 2 . As a result, the bulk CO 2 front becomes almost immobile. This implies that the caprock sealing capacity is unlikely to be compromised by a rapid capillary breakthrough and the injected CO 2 does not penetrate deep into the caprock. In the long term, the intrinsically slow molecular diffusion appears to dominate the migration of CO 2 dissolved into brine. Nonetheless, the inherently tortuous nature of shaly caprock further holds back the diffusive flow, favoring safe underground storage of CO 2 over geological time scales.

58 GEOSCIENCES↗

DOE OSTI2023

Stream lamination and rapid mixing in a microfluidic jet for X-ray spectroscopy studies

Microfluidic mixers offer new possibilities for the study of fast reaction kinetics down to the microsecond time scale, and methods such as soft X-ray absorption spectroscopy are powerful analysis techniques. These systems impose challenging constraints on mixing time scales, sample volume, detection region size and component materials. The current work presents a novel micromixer and jet device which aims to address these limitations. The system uses a so-called ‘theta’ mixer consisting of two sintered and fused glass capillaries. Sample and carrier fluids are injected separately into the inlets of the adjacent capillaries. At the downstream end, the two streams exit two micron-scale adjoining nozzles and form a single free-standing jet. The flow-rate difference between the two streams results in the rapid acceleration and lamination of the sample stream. This creates a small transverse dimension and induces diffusive mixing of the sample and carrier stream solutions within a time scale of 0.9 microseconds. The reaction occurs at or very near a free surface so that reactants and products are more directly accessible to interrogation using soft X-ray. We use a simple diffusion model and quantitative measurements of fluorescence quenching (of fluorescein with potassium iodide) to characterize the mixing dynamics across flow-rate ratios.

Huyke, Diego A. (ORCID:0000000283356613)↗

DOE OSTI2022

The effect of original and initial saturation on residual nonwetting phase capillary trapping efficiency

Injection of supercritical carbon dioxide (CO 2 ) into geological formations is a strategy for both atmospheric greenhouse gas reduction (climate change mitigation) and enhanced oil recovery. To understand CO 2 trapping efficiency, the capillary trapping behaviors that immobilize subsurface fluids were analyzed at the pore-scale using pairs of proxy fluids representing the range of in situ nonwetting and wetting fluid properties encountered in geologic storage reservoirs. The pairs of fluids were cycled through imbibition and drainage processes using a flow cell apparatus containing a sintered glass bead column. Computed x-ray microtomography (microCT) was used to identify immobilized nonwetting fluid after imbibition and drainage events. From microCT images, the trapped residual (post-secondary imbibition) nonwetting phase was spatially correlated to both the original (post-primary imbibition) and the initial (post-primary drainage) nonwetting phase; this relationship is referred to here as the original saturation dependence (SO-dependence) and initial saturation dependence (SI-dependence), respectively. Significant trends of decreasing SO- and SI-dependence with increasing wetting and nonwetting fluid phase viscosities were observed. This finding implies that the amount of CO 2 injected and ultimately trapped is dependent on the nonwetting phase (e.g. oil or gas) already present in the formation, as well as on the manner in which supercritical CO 2 is initially injected, which are factors not considered in current trapping models. To explore the potential effect that varying viscosity and interfacial tension (IFT) might have on this process, we report on a variety of fluid pairs with different viscosities and IFT.

42 ENGINEERING↗

DOE OSTI2022

Modified Lucas-Washburn theory for fluid filling in nanotubes

Ultrafast water transport in carbon nanotubes (CNTs) has drawn a great deal of attention in a number of applications, such as water desalination, power generation, and biomolecule detection. With the recent experimental advances in water filling of isolated CNTs, the Lucas-Washburn theory for capillary rise in tubes needs to be revisited for a better understanding of the physics and dynamics of water filling in CNTs. Here, the Lucas-Washburn theory is corrected for the hydrodynamic entrance effects as well as the variation of capillary pressure and hydrodynamic properties with the radius and length of CNTs. Due to the large slippage in CNTs, inclusion of the entrance effects is important particularly for the initial stages of filling where a L ∝ t scaling, as opposed to L 2 ∝ t , is observed in our molecular dynamics (MD) simulations. The corrected Lucas-Washburn theory is shown to predict the water filling dynamics in CNTs as observed in MD simulations. With the corrected theory, we achieve a better understanding of capillary rise and water filling dynamics in CNTs.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2021

Modeling and simulation of vascular tumors embedded in evolving capillary networks

Here in this work, we present a coupled 3D–1D model of solid tumor growth within a dynamically changing vascular network to facilitate realistic simulations of angiogenesis. Additionally, the model includes erosion of the extracellular matrix, interstitial flow, and coupled flow in blood vessels and tissue. We employ continuum mixture theory with stochastic Cahn–Hilliard type phase-field models of tumor growth. The interstitial flow is governed by a mesoscale version of Darcy’s law. The flow in the blood vessels is controlled by Poiseuille flow, and Starling’s law is applied to model the mass transfer in and out of blood vessels. The evolution of the network of blood vessels is orchestrated by the concentration of the tumor angiogenesis factors (TAFs); blood vessels grow towards the increasing TAFs concentrations. This process is not deterministic, allowing random growth of blood vessels and, therefore, due to the coupling of nutrients in tissue and vessels, makes the growth of tumors stochastic. We demonstrate the performance of the model by applying it to a variety of scenarios. Numerical experiments illustrate the flexibility of the model and its ability to generate satellite tumors. Simulations of the effects of angiogenesis on tumor growth are presented as well as sample-independent features of cancer.

3D–1D coupled blood flow models↗

DOE OSTI2020

Non-local model for surface tension in fluid-fluid simulations

We propose a non-local model for surface tension obtained in the form of an integral of a molecular-force-like function with support 3.5e added to the Navier-Stokes momentum conservation equation. We demonstrate analytically and numerically that with the non-local model interfaces with a radius of curvature larger than the support length behave macroscopically and microscopically, otherwise. For static droplets, the pressure difference Pe,in - Pe,out satisfies the Young-Laplace law for droplet radius greater than 3.5e and other- wise deviates from the Young-Laplace law. The latter indicates that the surface tension in the proposed model decreases with decreasing radius of curvature, which agrees with molecular dynamics and experimental studies of nanodroplets. Using the non-local model we perform numerical simulations of droplets under dynamic conditions, including a rising droplet, a droplet in shear flow, and two colliding droplets in shear flow, and compare results with a standard Navier-Stokes model subject to the Young-Laplace boundary condition at the fluid-fluid interface implemented via the Conservative Level Set (CLS) method. We find good agreement with existing numerical methods and analytical results for a rising macroscopic droplet and a droplet in a shear flow. For colliding droplets in shear flow, the non- local model converges (with respect to the grid size) to the correct behavior, including sliding, coalescence, and merging and breaking of two droplets depending on the capillary number. In contrast, we find that the results of the CLS model are highly grid-size dependent.

Howard, Amanda A.↗