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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Iodine effective diffusion coefficients through volcanic rock: Influence of iodine speciation and rock geochemistry

Accurate prediction of the subsurface transport of iodine species is important for the assessment of long-term nuclear waste repository performance, as well as monitoring compliance with the Comprehensive Nuclear-Test-Ban Treaty, given that radioiodine decays into radioxenon. However, the transport of iodine through intact geologic media is not well understood, compromising our ability to assess risk associated with radioiodine migration. The current study's goal is to quantify the matrix diffusion of iodine species through saturated volcanic rock, with particular attention paid to the redox environment and potential speciation changes. Here, diffusion experiments were run for iodide through lithophysae-rich lava, lithophysae-poor lava, and welded tuff, whereas iodate diffusion was studied through welded tuff. Iodine transport was compared with a conservative tracer, HDO, and effective diffusion coefficients were calculated. Likely due to a combination of size and anion exclusion effects, iodine species diffused more slowly than the conservative tracer through all rock types tested. Furthermore, oxidation of iodide to iodate was observed in the lithophysae-poor lava, affecting transport. Results provide much needed data for subsurface transport models that predict radioiodine migration from underground sources, and indicate the pressing need for geochemical and redox interactions to be incorporated into these models.

58 GEOSCIENCES↗
DOE OSTI2022

Closures for multicomponent reacting flows based on dispersion analysis

This work presents algebraic closure models associated with advective transport and nonlinear reactions in a Reynolds-averaged Navier-Stokes context for a system of species subject to binary reactions and transport by advection and diffusion. Expanding upon analysis originally developed for non-reactive transport in the context of Taylor dispersion of scalars, this work extends the modified gradient diffusion model explicated by Peters [N. Peters, Turbulent Combustion, Cambridge Monographs on Mechanics (Cambridge University Press, Cambridge, 2000)] and based on work by Corrsin [S. Corrsin, The reactant concentration spectrum in turbulent mixing with a first-order reaction, J. Fluid Mech. 11, 407 (1961)] beyond single-component transport phenomena and involving nonlinear reactions. The presented model forms, from this weakly nonlinear extension of the original dispersion theory, lead to an analytic expression for the eddy diffusivity matrix that explicitly captures the influence of the reaction kinetics on the closure operators. Furthermore, we demonstrate that the derived model form directly translates between flow topologies through a priori and a posteriori testing of a binary species system subject to homogeneous isotropic turbulence. Using two- and three-dimensional direct numerical simulations involving laminar and turbulent flows, it is shown that this framework improves prediction of mean quantities compared to previous results. Lastly, the presented model form, collapses to the earlier gradient diffusion and its modified version derived by Corrsin in the limits of nonreactive species and linear reactions, respectively.

42 ENGINEERING↗
DOE OSTI2017

Assessing Electrolyte Transport Properties with Molecular Dynamics

Here in this work we use estimates of ionic transport properties obtained from molecular dynamics to rank lithium electrolytes of different compositions. We develop linear response methods to obtain the Onsager diffusivity matrix for all chemical species, its Fickian counterpart, and the mobilities of the ionic species. We apply these methods to the well-studied propylene carbonate/ethylene carbonate solvent with dissolved LiBF 4 and O 2 . The results show that, over a range of lithium concentrations and carbonate mixtures, trends in the transport coefficients can be identified and optimal electrolytes can be selected for experimental focus; however, refinement of these estimation techniques is necessary for a reliable ranking of a large set of electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Regional-scale analysis of karst underground flow deduced from tracing experiments: examples from carbonate aquifers in Malaga province, southern Spain

Tracer concentration data from field experiments conducted in several carbonate aquifers (Malaga province, southern Spain) were analyzed following a dual approach based on the graphical evaluation method (GEM) and solute transport modeling to decipher flow mechanisms in karst systems at regional scale. The results show that conduit system geometry and flow conditions are the principal factors influencing tracer migration through the examined karst flow routes. Solute transport is mainly controlled by longitudinal advection and dispersion throughout the conduit length, but also by flow partitioning between mobile and immobile fluid phases, while the matrix diffusion process appears to be less relevant. The simulation of tracer breakthrough curves (BTCs) suggests that diffuse and concentrated flow through the unsaturated zone can have equivalent transport properties under extreme recharge, with high flow velocities and efficient mixing due to the high hydraulic gradients generated. Tracer mobilization within the saturated zone under low flow conditions mainly depends on the hydrodynamics (rather than on the karst conduit development), which promote a lower longitudinal advection and retardation in the tracer migration, resulting in a marked tailing effect of BTCs. The analytical advection-dispersion equation better approximates the effective flow velocity and longitudinal dispersion estimations provided by the GEM, while the non-equilibrium transport model achieves a better adjustment of most asymmetric and long-tailed BTCs. The assessment of karst underground flow properties from tracing tests at regional scale can aid design of groundwater management and protection strategies, particularly in large hydrogeological systems (i.e. transboundary carbonate aquifers) and/or in poorly investigated ones.

58 GEOSCIENCES↗
DOE OSTI2016

Investigating the age distribution of fracture discharge using multiple environmental tracers, Bedrichov Tunnel, Czech Republic

We investigated the transit time distribution (TTD) of discharge collected from fractures in the Bedrichov Tunnel, Czech Republic, using lumped parameter models and multiple environmental tracers. We then utilize time series of δ 18 O, δ 2 H and 3 H along with CFC measurements from individual fractures in the Bedrichov Tunnel of the Czech Republic to investigate the TTD, and the uncertainty in estimated mean travel time in several fracture networks of varying length and discharge. We also compare several TTDs, including the dispersion distribution, the exponential distribution, and a developed TTD which includes the effects of matrix diffusion. The effect of seasonal recharge is explored by comparing several seasonal weighting functions to derive the historical recharge concentration. We identify best fit mean ages for each TTD by minimizing the error-weighted, multi-tracer χ2 residual for each seasonal weighting function. We use this methodology to test the ability of each TTD and seasonal input function to fit the observed tracer concentrations, and the effect of choosing different TTD and seasonal recharge functions on the mean age estimation. We find that the estimated mean transit time is a function of both the assumed TTD and seasonal weighting function. Best fits as measured by the χ2 value were achieved for the dispersion model using the seasonal input function developed here for two of the three modeled sites, while at the third site, equally good fits were achieved with the exponential model and the dispersion model and our seasonal input function. The average mean transit time for all TTDs and seasonal input functions converged to similar values at each location. The sensitivity of the estimated mean transit time to the seasonal weighting function was equal to that of the TTD. These results indicated that understanding seasonality of recharge is at least as important as the uncertainty in the flow path distribution in fracture networks and that unique identification of the TTD and mean transit time is difficult given the uncertainty in the recharge function. But, the mean transit time appears to be relatively robust to the structural model uncertainty. The results presented here should be applicable to other studies using environmental tracers to constrain flow and transport properties in fractured rock systems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Field experiments of surface water to groundwater recharge to characterize the mobility of uranium and vanadium at a former mill tailing site

Characterizing the mobility of uranium and vanadium in groundwater with a hydraulic connection to surface water is important to inform the best management practices of former mill tailing sites. In this study, the recharge of river water to the unsaturated and saturated zones of a uranium-contaminated alluvial aquifer was simulated in a series of forced-gradient single- and multi-well injection-extraction tests. The injection fluid (river water) was traced with natural and artificial tracers that included halides, fluorobenzoates, lithium, and naphthalene sulfonate to characterize the potential mass transport mechanisms of uranium and vanadium. The extraction fluid (river water/groundwater mixture) was analyzed for the tracers, uranium, and vanadium. The results from the tracers indicated that matrix diffusion was likely negligible over the spatiotemporal scales of the tests as evident by nearly identical breakthrough curves of the halides and fluorobenzoates. In contrast, the breakthrough curves of lithium and naphthalene sulfonate indicated that sorption by cation exchange and sorption to organic matter, respectively, were potential mass transport mechanisms of uranium and vanadium. Uranium was mobilized in the saturated zone containing gypsum (gypsum-rich zone), the vadose zone (vadose-rich zone), and the saturated zone containing organic carbon (organic-rich zone) whereas vanadium was mobilized only in the saturated gypsum-rich zone. The mechanisms responsible for the mobilization of uranium and vanadium were likely dissolution of uranium- and vanadium-bearing minerals and/or desorption from the gypsum-rich zone, flushing of uranium from the vadose-rich zone, and desorption of uranium from the organic-rich zone due to the natural contrast in the geochemistry between the river water and groundwater. The experimental design of this study was unique in that it employed the use of multiple natural and artificial tracers coupled with a direct injection of native river water to groundwater. Here, these results demonstrated that natural recharge and flooding events at former mill tailing sites can mobilize uranium, and possibly vanadium, and contribute to persistent levels of groundwater contamination.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

A comparative study of discrete fracture network and equivalent continuum models for simulating flow and transport in the far field of a hypothetical nuclear waste repository in crystalline host rock

One of the major challenges of simulating flow and transport in the far field of a geologic repository in crystalline host rock is related to reproducing the properties of the fracture network over the large volume of rock with sparse fracture characterization data. Various approaches have been developed to simulate flow and transport through the fractured rock. The approaches can be broadly divided into Discrete Fracture Network (DFN) and Equivalent Continuum Model (ECM). The DFN explicitly represents individual fractures, while the ECM uses fracture properties to determine equivalent continuum parameters. In this paper, we compare DFN and ECM in terms of upscaled observed transport properties through generic fracture networks. The major effort was directed on making the DFN and ECM approaches similar in their conceptual representations. This allows for separating differences related to the interpretation of the test conditions and parameters from the differences between the DFN and ECM approaches. The two models are compared using a benchmark test problem that is constructed to represent the far field (1 × 1 × 1 km 3 ) of a hypothetical repository in fractured crystalline rock. The test problem setting uses generic fracture properties that can be expected in crystalline rocks. The models are compared in terms of the: 1) effective permeability of the domain, and 2) nonreactive solute breakthrough curves through the domain. The principal differences between the models are mesh size, network connectivity, matrix diffusion and anisotropy. We demonstrate how these differences affect the flow and transport. Finally, we identify the factors that should be taken in consideration when selecting an approach most suitable for the site-specific conditions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

PLUMECALC, Version 2.3.x

PLUMECALC is a post processor to random walk particle tracking simulations of subsurface solute transport. PLUMECALC takes results of a single particle tracking run without retention processes and incorporates the effects of matrix diffusion or other retention processes for a user-specified solute source.

Dash, Zora↗
DOE OSTI2019

Numerical Evaluation of Unsaturated-Zone Flow and Transport Pathways at Rainier Mesa, Nevada

Sixty-one underground nuclear tests were conducted at Rainier Mesa at the Nevada National Security Site between 1957 and 1992. The mesa includes the highest-elevation areas at the Nevada National Security Site and experiences some of the highest estimated infiltration rates. Perched water is ubiquitous in many of the tunnels used for testing. The presence of sloping layers with strongly varying degrees of fracturing and overall permeability suggests that some infiltrating water may be diverted laterally along higher-permeability layers, thereby reducing overall percolation flux and radionuclide transport through the low-permeability testing horizons but also potentially transporting radionuclides laterally away from the test locations. A high-resolution, two-dimensional, cross-sectional model was created to simulate water and particle movement along potential lateral flow paths and to investigate flow and transport paths within and surrounding the perched water bodies. The model results indicate that particles with starting locations within the low-permeability perching layers will follow dominantly vertical trajectories through the perching horizons and reach the water table in the underlying carbonate aquifer only after many thousands of years. In contrast, particles starting near ground surface above the testing horizon are mostly diverted laterally before reaching the testing horizon, except where nearby faults through the perching layers are present. Where the rock above the perching horizon is fractured, particles originating near ground surface can move laterally with relatively high transport velocities. Transport calculations for 3 H show that transport extent is limited by slow matrix flow, radioactive decay, and matrix diffusion in the fractured units.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Dissolved Organic Carbon 14C in Southern Nevada Groundwater and Implications for Groundwater Travel Times

Dissolved inorganic carbon (DIC) carbon-14 ( 14 C) ages must be corrected for complex chemical and physical reactions and processes that change the amount of 14 C in groundwater as it flows from recharge to downgradient areas. Because of these reactions, DIC 14 C can produce unrealistically old ages and long groundwater travel times that may, or may not, agree with travel times estimated by other methods. Dissolved organic carbon (DOC) 14 C ages are often younger than DIC 14 C ages because there are few chemical reactions or physical processes that change the amount of DOC 14 C in groundwater. However, there are several issues that create uncertainty in DOC 14 C groundwater ages including limited knowledge of the initial (A 0 ) DOC 14 C in groundwater recharge and potential changes in DOC composition as water moves through an aquifer. This study examines these issues by quantifying A 0 DOC 14 C in recharge areas of southern Nevada groundwater flow systems and by evaluating changes in DOC composition as water flows from recharge areas to downgradient areas. The effect of these processes on DOC 14 C groundwater ages is evaluated and DOC and DIC 14 C ages are then compared along several southern Nevada groundwater flow paths. Twenty-seven groundwater samples were collected from springs and wells in southern Nevada in upgradient, midgradient, and downgradient locations. DOC 14 C for upgradient samples ranged from 96 to 120 percent modern carbon (pmc) with an average of 106 pmc, verifying modern DOC 14 C ages in recharge areas, which decreases uncertainty in DOC 14 C A 0 values, groundwater ages, and travel times. The HPLC spectra of groundwater along a flow path in the Spring Mountains show the same general pattern indicating that the DOC compound composition does not change along this flow path. Although DOC concentration decreases from recharge-area to downgradient groundwater, the organic compounds are similar, indicating that DOC 14 C is unaffected by other processes such as microbial degradation. A small amount of organic carbon was leached from crushed volcanic and carbonate aquifer outcrop rock in rock-leaching experiments. The leached DOC was high in 14 C (75 pmc carbonate rocks, 91 pmc volcanic) suggesting that the leached DOC likely came from microbes in the rock samples. The small amount of DOC and high 14 C indicates that the amount of old organic carbon in these rocks is low so there should be minimal impact on groundwater DOC 14 C ages. Based on the results from this study, DOC 14 C ages do not require additional corrections. Several correction models were applied to DIC 14 C ages to correct for water-rock reactions along two carbonate and two volcanic flow paths and the corresponding travel times were compare to DOC 14 C travel times. The DOC 14 C travel times were hundreds to thousands of years shorter than uncorrected and corrected DIC 14 C travel times except for the upper section of one carbonate flow path. DOC 14 C travel times ranged from 400 to 5,400 years as compared to DIC 14 C that ranged from modern to 20,900 years. The DIC 14 C ages are greatly influenced by carbonate mineral and gas reactions and other processes such as matrix diffusion, isotope exchange, or adsorption, which are not always adequately accounted for in DIC 14 C groundwater age correction models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Preliminary Interpretations from Fall 2018 Field Test at Ne’ot Hovav

Presentation conclusions: Conservative tracer transport was reasonably consistent with earlier tests between RH11c and RH11a; No attempt to model bentonite colloids because of minimal elevation of Al concentrations over background; Modeling confirms what we knew already for Cs and Ce; Cs transports as solute that sorbs in matrix (after diffusion into matrix); Ce transports as colloid that is rapidly filtered; Sr not modeled, but qualitatively appears consistent with combination of colloid and solute transport

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Approximate solutions for diffusive fracture-matrix transfer: Application to storage of dissolved CO 2 in fractured rocks

Analytical solutions with infinite exponential series are available to calculate the rate of diffusive transfer between low-permeability blocks and high-permeability zones in the subsurface. Truncation of these series is often employed by neglecting the early-time regime. Here in this paper, we present unified-form approximate solutions in which the early-time and the late-time solutions are continuous at a switchover time. The early-time solutions are based on three-term polynomial functions in terms of square root of dimensionless time, with the first coefficient dependent only on the dimensionless area-to-volume ratio. The last two coefficients are either determined analytically for isotropic blocks (e.g., spheres and slabs) or obtained by fitting the exact solutions, and they solely depend on the aspect ratios for rectangular columns and parallelepipeds. For the late-time solutions, only the leading exponential term is needed for isotropic blocks, while a few additional exponential terms are needed for highly anisotropic rectangular blocks. The optimal switchover time is between 0.157 and 0.229, with highest relative approximation error less than 0.2%. The solutions are used to demonstrate the storage of dissolved CO 2 in fractured reservoirs with low-permeability matrix blocks of single and multiple shapes and sizes. These approximate solutions are building blocks for development of analytical and numerical tools for hydraulic, solute, and thermal diffusion processes in low-permeability matrix blocks.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Structural deformation and transformation of θ'-Al 2 Cu precipitate in Al matrix via interfacial diffusion

Metastable θ'-Al 2 Cu precipitates enhance mechanical properties of Al alloy, but gradually transform to θ phase due to diffusion related coarsening at higher temperatures (>200°C). To improve understanding of the phase instability and transformation of θ'-Al 2 Cu, we investigated the interfacial atomic mobility of θ'-Al2Cu precipitate in Al matrix via molecular dynamics (MD). To characterize the interfacial atomic mobility, diffusion properties (activation energy, diffusivity, and jump attempt frequency) with respect to atomic species, interfacial structure, and temperature are calculated using atomic trajectories from MD. For the enhanced accuracy of this analysis, especially at low temperatures, temporal scale of molecular dynamics is significantly extended by employing the parallel replica dynamics. This study, as the first MD investigation on atomic diffusion of θ'-Al 2 Cu in Al matrix, suggests and discusses (i) structural deformation activated at the semi-coherent θ'-Al 2 Cu/Al interfaces, (ii) transformation initiated at the edge of the coherent θ'-Al 2 Cu/Al interface, and (iii) directional dependence of diffusion properties. Overall, these findings are expected to be employed in a larger scale phase-field modeling of precipitate growth, and to contribute to the understanding of phase transformation process and the development of alloys with θ'-phase retained to higher temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Self-similar solutions for multi-species plasma mixing by gradient driven transport

We report that multi-species transport of plasma ions across an initial interface between DT and CH is shown to exhibit self-similar species density profiles under 1D isobaric conditions. Results using transport theory from recent studies and using a Maxwell–Stephan multi-species approximation are found to be in good agreement for the self-similar mix profiles of the four ions under isothermal and isobaric conditions. The individual ion species mass flux and molar flux profile results through the mixing layer are examined using transport theory. The sum over species mass flux is confirmed to be zero as required, and the sum over species molar flux is related to a local velocity divergence needed to maintain pressure equilibrium during the transport process. The light ion species mass fluxes are dominated by the diagonal coefficients of the diffusion transport matrix, while for the heaviest ion species (C in this case), the ion flux with only the diagonal term is reduced by about a factor two from that using the full diffusion matrix, implying the heavy species moves more by frictional collisions with the lighter species than by its own gradient force. Temperature gradient forces were examined by comparing profile results with and without imposing constant temperature gradients chosen to be of realistic magnitude for ICF experimental conditions at a fuel-capsule interface (10 μm scale length or greater). The temperature gradients clearly modify the relative concentrations of the ions, for example near the fuel center, however the mixing across the fuel-capsule interface appears to be minimally influenced by the temperature gradient forces within the expected compression and burn time. Finally, discussion considers the application of the self-similar profiles to specific conditions in ICF.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Characterizing the impact of finite matrix block size on conservative particle transport through three-dimensional fracture networks

Mass transfer of solutes between fractures and the surrounding rock matrix exerts a noticeable signature on the tail of travel time distributions. When the width of the matrix is assumed to be infinite and advective transport through the fracture is sufficiently fast, the tails of the travel time distributions exhibit a classically expected slope of ψ(t) ∝ t -3/2 . However, studies have yet to characterize how solute transfer between fractures via diffusion through finite matrix blocks influences the tail’s slope in three-dimensional fractured media. Here, in this study, we assess the impact of finite matrix block size on breakthrough curve shape at different spatio-temporal scales by con ducting particle tracking simulations in three-dimensional discrete fracture networks. We consider a variety of hydrodynamic and geostructural proper ties to determine their relative impact on the resulting travel time distributions. We observe that the impact of matrix diffusion through a finite block on travel time distributions is similar to that of an infinite matrix block when the fracture spacing is sufficiently large, matrix diffusion is relatively weak, or transport is considered at an early control plane distance. We observe that the converse of these conditions, results in deviations from the classical ψ(t) ∝ t -3/2 scaling. These results provide a first step toward developing a metric to assess when finite block size effects are expected to significantly influence transport.

58 GEOSCIENCES↗
DOE OSTI2024

Patch2Self2: Self-supervised Denoising on Coresets via Matrix Sketching

Diffusion MRI (dMRI) non-invasively maps brain white matter yet necessitates denoising due to low signal-to-noise ratios. Patch2Self (P2S) employing self-supervised techniques and regression on a Casorati matrix effectively denoises dMRI images and has become the new de-facto standard in this field. P2S however is resource intensive both in terms of running time and memory usage as it uses all voxels (n) from all-but-one held-in volumes (d-1) to learn a linear mapping Phi : \mathbb R ^ n x(d-1) \mapsto \mathbb R ^ n for denoising the held-out volume. The increasing size and dimensionality of higher resolution dMRI acquisitions can make P2S infeasible for large-scale analyses. This work exploits the redundancy imposed by P2S to alleviate its performance issues and inspect regions that influence the noise disproportionately. Specifically this study makes a three-fold contribution: (1) We present Patch2Self2 (P2S2) a method that uses matrix sketching to perform self-supervised denoising. By solving a sub-problem on a smaller sub-space so called coreset we show how P2S2 can yield a significant speedup in training time while using less memory. (2) We present a theoretical analysis of P2S2 focusing on determining the optimal sketch size through rank estimation a key step in achieving a balance between denoising accuracy and computational efficiency. (3) We show how the so-called statistical leverage scores can be used to interpret the denoising of dMRI data a process that was traditionally treated as a black-box. Experimental results on both simulated and real data affirm that P2S2 maintains denoising quality while significantly enhancing speed and memory efficiency achieved by training on a reduced data subset.

Fadnavis, Shreyas↗
DOE OSTI2021

Coordinatively and Spatially Coconfining High-Loading Atomic Sb in Sulfur-Rich 2D Carbon Matrix for Fast K + Diffusion and Storage

The atomically dispersed materials promise ultrafast redox kinetics for alkali-ion storage. However, their relatively low mass loading limits their application. In this work, well-dispersed Sb atoms with high-loading of 23.3 wt % anchored in sulfur-rich amorphous carbon-coated reduced graphene oxide matrix (SbSA/C) are prepared by a coordinative and spatial coconfinement methodology including freeze-casting the well-dissolved Sb-chelates (Sb-thioglycolate) within graphene oxide suspension and post heating-treatment. The reduced graphene oxide substrate features open two-dimensional spatial framework for loading atomically dispersive Sb species, and the pyrolyzed Sb-chelates would provide not only massive desirable heteroatoms (S, O) for coordinating the Sb atoms but also in situ pyrolytic carbon for further spatially separating those dispersive atoms. The coordinative and spatial coconfinement engineering also endows the SbSA/C composite with atomic-level Sb atoms against migration and agglomeration during electrochemical K-storage cycling. In situ TEM reveals the uniform potassiation behavior of the SbSA/C without obvious volume change; DFT calculation and electrochemical characterization suggest the significantly lower K-ion diffusion energy barrier. Therefore, on the basis of both the active Sb center and the coordinative heteroatom, the SbSA/C electrode delivers high fast-charging capacity, outstanding rate capability and long-lifespan performance in half/full K-ion batteries (e.g., a stable capacity of 331.3 mA h g –1 is maintained over 1100 cycles at 1.0 A g –1 for half-cell).

36 MATERIALS SCIENCE↗