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All sources NASA NTRS DOE OSTI

DOE OSTI2023

Understanding capacity fade in organic redox-flow batteries by combining spectroscopy with statistical inference techniques

Organic redox-active molecules are attractive as redox-flow battery (RFB) reactants because of their low anticipated costs and widely tunable properties. Unfortunately, many lab-scale flow cells experience rapid material degradation (from chemical and electrochemical decay mechanisms) and capacity fade during cycling (>0.1%/day) hindering their commercial deployment. In this work, we combine ultraviolet-visible spectrophotometry and statistical inference techniques to elucidate the Michael attack decay mechanism for 4,5-dihydroxy-1,3-benzenedisulfonic acid (BQDS), a once-promising positive electrolyte reactant for aqueous organic redox-flow batteries. We use Bayesian inference and multivariate curve resolution on the spectroscopic data to derive uncertainty-quantified reaction orders and rates for Michael attack, estimate the spectra of intermediate species and establish a quantitative connection between molecular decay and capacity fade. Our work illustrates the promise of using statistical inference to elucidate chemical and electrochemical mechanisms of capacity fade in organic redox-flow battery together with uncertainty quantification, in flow cell-based electrochemical systems.

25 ENERGY STORAGE↗

DOE OSTI2020

Imaging viscous flow of the Dirac fluid in graphene

The electron–hole plasma in charge-neutral graphene is predicted to realize a quantum critical system in which electrical transport features a universal hydrodynamic description, even at room temperature. This quantum critical ‘Dirac fluid’ is expected to have a shear viscosity close to a minimum bound, with an interparticle scattering rate saturating1 at the Planckian time, the shortest possible timescale for particles to relax. Although electrical transport measurements at finite carrier density are consistent with hydrodynamic electron flow in graphene a clear demonstration of viscous flow at the charge-neutrality point remains elusive. In this work, we directly image viscous Dirac fluid flow in graphene at room temperature by measuring the associated stray magnetic field. Nanoscale magnetic imaging is performed using quantum spin magnetometers realized with nitrogen vacancy centres in diamond. Scanning single-spin and wide-field magnetometry reveal a parabolic Poiseuille profile for electron flow in a high-mobility graphene channel near the charge-neutrality point, establishing the viscous transport of the Dirac fluid. This measurement is in contrast to the conventional uniform flow profile imaged in a metallic conductor and also in a low-mobility graphene channel. Furthermore, via combined imaging and transport measurements, we obtain viscosity and scattering rates, and observe that these quantities are comparable to the universal values expected at quantum criticality. This finding establishes a nearly ideal electron fluid in charge-neutral, high-mobility graphene at room temperature4. Our results will enable the study of hydrodynamic transport in quantum critical fluids relevant to strongly correlated electrons in high-temperature superconductors9. This work also highlights the capability of quantum spin magnetometers to probe correlated electronic phenomena at the nanoscale.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2026

Differentiable multiphase flow model for physics-informed machine learning in reservoir pressure management

Accurate subsurface reservoir pressure control is extremely challenging due to geological heterogeneity and multiphase fluid-flow dynamics. Predicting behavior in this setting relies on high-fidelity physics-based simulations that are computationally expensive. Yet, the uncertain, heterogeneous properties that control these flows make it necessary to perform many of these expensive simulations, which is often prohibitive. To address these challenges, we introduce a physics-informed machine learning workflow that couples a fully differentiable multiphase flow simulator, which is implemented in the DPFEHM framework with a convolutional neural network (CNN). The CNN learns to predict fluid extraction rates from heterogeneous permeability fields to enforce pressure limits at critical reservoir locations. By incorporating transient multiphase flow physics into the training process, our method enables more practical and accurate predictions for realistic injection-extraction scenarios compared to previous works. To speed up training, we pretrain the model on single-phase, steady-state simulations and then finetune it on full multiphase scenarios, which dramatically reduces the computational cost. We demonstrate that high-accuracy training can be achieved with fewer than three thousand full-physics multiphase flow simulations – compared to previous estimates requiring up to ten million. This drastic reduction in the number of simulations is achieved by leveraging transfer learning from much less expensive single phase simulations.

25 ENERGY STORAGE↗

DOE OSTI2020

Evaluating aqueous flow battery electrolytes: a coordinated approach

Here, we outline some basic pitfalls in the electrochemical investigation of aqueous metal complexes and advocate for the use of bulk electrolysis in redox flow cells for electrolyte analysis. We demonstrate the methods of operation and performance of a lab scale redox flow battery (RFB), which is assembled from unmodified, commercially available material and cycled with a vanadium electrolyte in order to provide a comparative baseline of expected performance. Common misconceptions about the thermodynamic window for water splitting are addressed and further express the need to develop next-generation aqueous redox flow battery electrolytes. Although non-aqueous electrolytes are a popular approach, they suffer from distinct challenges that limit energy and power density in comparison with aqueous electrolytes. Expanding the scope of aqueous electrolytes to include metal–chelate complexes allows electrolytes to be as tailorable as organic species, while maintaining robust metal-based redox processes. A flow battery assembly and operation guide is provided to help facilitate the use of flow battery testing in the evaluation of next-generation electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Flow synthesis of iron oxide nanoparticles: using multiple precursor additions to improve size control

Controlling the size of iron oxide nanoparticles while maintaining uniformity in flow-based synthesis systems has been a great challenge in nanoparticle synthesis. Using an extended LaMer mechanism, we improve both the size and shape uniformity as compared to a conventional flow synthesis. The key to this approach is the injection of additional Fe precursor during the flow reaction, providing extra precursor during the growth process leading to a size focusing step. This approach has also allowed for the systematic variation of the nanoparticle size produced in the flow reaction. This work represent a new synthetic concept for improving the size uniformity of iron oxide nanoparticles in flow-based synthesis and has potential for application across a wide range of nanoparticle systems.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Computational fluid dynamics analysis of char conversion in Sandia’s pressurized entrained flow reactor

Design and analysis of practical reactors utilizing solid feedstocks rely on reaction rate parameters that are typically generated in lab-scale reactors. Evaluation of the reaction rate information often relies on assumptions of uniform temperature, velocity, and species distributions in the reactor, in lieu of detailed measurements that provide local information. This assumption might be a source of substantial error, since reactor designs can impose significant inhomogeneities, leading to data misinterpretation. Spatially resolved reactor simulations help understand the key processes within the reactor and support the identification of severe variations of temperature, velocity, and species distributions. In this work, Sandia’s pressurized entrained flow reactor is modeled to identify inhomogeneities in the reaction zone. Tracer particles are tracked through the reactor to estimate the residence times and burnout ratio of introduced coal char particles in gasifying environments. The results reveal a complex mixing environment for the cool gas and particles entering the reactor along the centerline and the main high-speed hot gas reactor flow. Furthermore, the computational fluid dynamics (CFD) results show that flow asymmetries are introduced through the use of a horizontal gas pre-heating section that connects to the vertical reactor tube. Computed particle temperatures and residence times in the reactor differ substantially from the idealized plug flow conditions typically evoked in interpreting experimental measurements. Furthermore, experimental measurements and CFD analysis of heat flow through porous refractory insulation suggest that for the investigated conditions (1350 °C, <20 atm), the thermal conductivity of the insulation does not increase substantially with increasing pressure.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Experimental investigation of internal two-phase flow structures and dynamics of quasi-stable sheet cavitation by fast synchrotron x-ray imaging

The quasi-stable sheet cavitation produced in a small Venturi channel is investigated using a fast synchrotron X-ray imaging technique aided with conventional high speed photography. The use of X-rays instead of visible light solves cavitation opacity related issues, and X-ray phase contrast-based edge enhancement enables high-definition visualization of the internal two-phase morphology. The simultaneous acquisition of time-resolved velocity and void fraction fields through post-processing the recorded X-ray images reveals, for the first time, the complex diphasic flow structures inside the sheet cavity, which is essentially divided into 6 characteristic parts. Distinct from the current mainstream view, the globallysteady sheet cavitation is found to be characterized by a weak but constantly-existing re-entrant flow that can penetrate the entire cavity. The turbulent velocity fluctuations inside the sheet cavity are also investigated. The turbulence level in the reverse flow region is observed to be as low as in the outer main flow demonstrating the relatively steady status of the reentrant flow. Unlike the streamwise and cross-stream fluctuations, the shear stress appears to be weakly correlated with the velocity gradient. The collapse of vapor phase and the vaporization at the upstream cavity interface are found to be the primary causes of shear stress intensification.

42 ENGINEERING↗

DOE OSTI2021

Role of deep levels and barrier height lowering in current-flow mechanism in 150 μ m thick epitaxial n-type 4H–SiC Schottky barrier radiation detectors

Schottky barrier detectors (SBDs) require larger surface areas than conventional electronics to increase the detection efficiency although such SBDs manifest large diode ideality factors due to inhomogeneous areal distribution of surface barrier height (SBH). Inhomogeneous SBH distributions lead to various current flow mechanisms in SBDs, which need to be identified to optimize detector performance. In this Letter, we identify the current flow mechanism in large area Schottky barrier diodes for radiation detection fabricated on 150 μm thick n-4H–SiC epitaxial layers. The analysis of temperature-dependent forward current–voltage (I–V–T) characteristics of SBDs revealed two linear regions in current–voltage curves up to 450 K, one corresponding to the current flow through a low barrier patch, while the other corresponds to that of average barrier distribution. Applying a SBH distribution model to the reverse I–V–T characteristics, an activation energy of 0.76 eV for the current flow over the Schottky barrier was calculated. Additionally, the activation energy did not directly correspond to any of the defect levels observed from the deep level transient spectroscopy (DLTS). Above 450 K, a Schottky type barrier lowering suggested a current flow through a low barrier patch of ≈ 0.8 eV. The absence of any SBH lowering below 450 K indicated that the current corresponded to a neutrally charged trap level at ≈ 0.6 eV below the conduction band edge, which was consistent with DLTS measurements revealing the presence of an electron trap level Z1/2 at 0.59 eV below the conduction band edge.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Relativistic wind farm effect: Possibly turbulent flow of a charged, massless relativistic fluid in graphene

At low Reynolds numbers, the wind flow in the wake of a single wind turbine is generally not turbulent. However, turbines in wind farms affect each other's wakes so that a turbulent flow can arise. In the present work, an analog of this effect for the massless charge carrier flow around obstacles in graphene is outlined. We use a relativistic hydrodynamic simulation to analyze the flow in a sample containing impurities. Depending on the density of impurities in the sample, we indeed find evidence for potentially turbulent flow and discuss experimental consequences.

Watson, Mark (ORCID:0000000258959949)↗

DOE OSTI2022

Large eddy simulation of flow through an axisymmetric sudden expansion

Here, this study aims at investigating the inlet flow conditions of flow through an axisymmetric sudden expansion with an expansion ratio of 2.0. A series of large eddy simulations with the WALE model were conducted for different inlet Reynolds numbers ( Re) and turbulence intensities ($u_{rms}/\bar{U}_m$). The reattachment length, defined as the length measured downstream of the expansion where the flow direction is reversed adjacent to the wall ( Lr), was measured for each case. For widely studied inlet turbulence intensity values (TI), the simulation results are in good agreement with the experimental and numerical results reported in the literature. Parametric studies revealed that turbulence intensity affects the critical Reynolds number, marking the transition between the laminar and transition regions and the reattachment length. The critical Reynolds number was found to decrease with increasing turbulence intensity. A correlation expression is proposed. Additional analysis with proper orthogonal decomposition was performed to enhance the understanding of complex flow structures downstream of the expansion. Finally, an overall correlation expression for the reattachment length was obtained for 500 ≤ Re ≤15 000 and 0.2 ≤ TI (%) ≤ 20. For a given turbulence intensity, the reattachment length can be expressed for laminar and turbulent regions as a function of the Reynolds number. The reattachment length in the transition region can be expressed as a fractional average of reattachment lengths for laminar and turbulent flows.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2024

Shock formation in flowing plasmas by temporally and spatially smoothed laser beams

The cumulative impact of multiple laser speckles on a supersonic plasma flow across optically smoothed laser beams is investigated. The bending of laser beams caused by ponderomotive laser–plasma coupling, together with flow, leads to plasma a momentum-conserving response that results in a deceleration of the flow. Once the flow velocity decreases to a subsonic level, the action of the laser beams can generate a shock within the plasma. This scenario has been predicted theoretically and confirmed by hydrodynamic simulations. The conditions of shock generation are given in terms of the ponderomotive pressure, speckle size, and the flow velocity. The nonlinear properties of the shocks are analyzed using Rankine–Hugoniot relations. According to linear theory, temporally smoothed beams exhibit a higher threshold for shock generation. Numerical simulations with beams that are smoothed by spectral dispersion compare well with the linear theory results, diverging only in the nonlinear regime. The conditions necessary for shock generation and their effects on the laser–plasma coupling in the inertial confinement fusion experiments are also discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Predicting turbulent wake flow of marine hydrokinetic turbine arrays in large-scale waterways via physics-enhanced convolutional neural networks

We present a physics-enhanced convolutional neural network (PECNN) algorithm for reconstructing the mean flow and turbulence statistics in the wake of marine hydrokinetic (MHK) turbine arrays installed in large-scale meandering rivers. The algorithm embeds the mass and momentum conservation equations into the loss function of the PECNN algorithm to improve the physical realism of the reconstructed flow fields. The PECNN is trained using large eddy simulation (LES) results of the wake flow of a single row of turbines in a virtual meandering river. Subsequently, the trained PECNN is applied to predict the wake flow of MHK turbines with arrangements and positionings different than those considered during the training process. The PECNN predictions are validated using the results of separately performed LES. The results show that the PECNN algorithm can accurately predict the wake flow of MHK turbine farms at a small fraction of the cost of LES. The PECNN can improve the accuracy by around 1% and reduce the physical constraint indices by around 50% compared to the CNN without physical constraints. This work underscores the potential of PECNN to develop reduced-order models for control co-design and optimization of MHK turbine arrays in natural riverine environments.

Mechanics↗

DOE OSTI2025

Measurement of near- and far-field impurity flows during pellet-induced rapid shutdown in DIII-D

Both near-field (<1 m away toroidally from the pellet) and far-field (>1 m away toroidally from the pellet) poloidal and toroidal impurity (carbon ion) flows are measured using visible imaging and fast bolometry during a polypropylene pellet-induced rapid plasma shutdown in the DIII-D tokamak. In the near field, the pellet appears to increase poloidal flow in the ion diamagnetic direction, possibly due to the strong radial temperature gradient caused by the pellet ablation. In the far field, the poloidal impurity flow typically appears slower and in the opposite direction. Toroidal impurity flow appears to be strongly influenced by the plasma initial toroidal rotation, especially in the far field. These results demonstrate that rapid shutdown impurity flows are not necessarily global in structure but can be quite different close to and far from the injected pellet.

Electromagnetic radiation detectors↗

DOE OSTI2024

Quantifying electron transport in aggregated colloidal suspensions in the strong flow regime

Electron transport in complex fluids, biology, and soft matter is a valuable characteristic in processes ranging from redox reactions to electrochemical energy storage. These processes often employ conductor–insulator composites in which electron transport properties are fundamentally linked to the microstructure and dynamics of the conductive phase. While microstructure and dynamics are well recognized as key determinants of the electrical properties, a unified description of their effect has yet to be determined, especially under flowing conditions. In this work, the conductivity and shear viscosity are measured for conductive colloidal suspensions to build a unified description by exploiting both recent quantification of the effect of flow-induced dynamics on electron transport and well-established relationships between electrical properties, microstructure, and flow. These model suspensions consist of conductive carbon black (CB) particles dispersed in fluids of varying viscosities and dielectric constants. In a stable, well-characterized shear rate regime where all suspensions undergo self-similar agglomerate breakup, competing relationships between conductivity and shear rate were observed. To account for the role of variable agglomerate size, equivalent microstructural states were identified using a dimensionless fluid Mason number, Mn f , which allowed for isolation of the role of dynamics on the flow-induced electron transport rate. At equivalent microstructural states, shear-enhanced particle–particle collisions are found to dominate the electron transport rate. This work rationalizes seemingly contradictory experimental observations in literature concerning the shear-dependent electrical properties of CB suspensions and can be extended to other flowing composite systems.

Science & Technology - Other Topics↗

DOE OSTI2021

Filamentary surface plasma discharge flow length and time scales

Nanosecond surface dielectric barrier discharges (ns-SDBDs) are a class of plasma actuators that utilize a high-voltage pulse of nanosecond duration between two surface-mounted electrodes to create an electrical breakdown of air, along with rapid heating. These actuators usually produce multiple filaments when operated at high pulse frequencies, and the rapid heating leads to the formation of shock waves and complex flow fields. In this work we replicate a single filament of the ns-SDBDs and characterize the induced flow using velocity measurements from particle image velocimetry and density measurements from background-oriented schlieren. The discharge is produced by a high voltage electrical pulse between two copper electrodes on an acrylic base. A hot gas kernel characterizes the flow field formed close to the electrodes that expands and cools over time and a vortex ring that propagates away from the surface while entraining cold ambient fluid. The gas density deficit inside the kernel displays a power-law decay over time. Based on the observations, we develop a simplified theoretical model based on vortex-driven cooling and perform a scaling analysis to obtain the induced flow length and time scales. The results show that the cooling process's time scales correspond to a circulation-based time scale of the vortex ring, and the length scale of the kernel corresponds to the vortex ring radius. Furthermore, these findings can guide the choice of optimal filament spacing and pulse frequencies in the design, deployment, and operation of ns-SDBDs for flow control.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Effect of parallel flow on resonant layer responses in high beta plasmas

Abstract Resonant layers in a tokamak respond to non-axisymmetric magnetic perturbations by amplifying the mode amplitude and balancing the plasma rotation through magnetic reconnection and force balance, respectively. This resonant response can be characterized by local layer parameters and especially by a single quantity in the linear regime, the so-called inner-layer Δ. The computation of Δ under two-fluid drift-MHD formalism has been progressed by reducing the order of the system in the phase space, where the shielding current is approximated as being only carried by electrons, a posteriori . In this study, we relax the approximation and compute Δ accounted for by the parallel flow associated with the ion shielding current. The posteriori is numerically verified in great agreement with the original SLAYER developed in a previous paper (J.-K. Park 2022 Phys. Plasmas 29 072506). Extending the resonant layer response theory to high β plasmas, our research findings answer two important questions: how the parallel flow influences the resonant layer response and why the parallel flow effect appears in high β plasmas. The complicated plasma compression in high β regime allows the parallel flow response to give rise to the ion shielding current, which not only shifts the zero-crossing condition of the ExB flow but also enhances the field penetration threshold. Technically, the Riccati matrix transformation method is adapted to handle the numerical stiffness due to the increased order of the system. The high fidelity of this numerical method makes use of further extension of the model to higher-order systems to take other physical phenomena into account. This work is envisaged to predict the resonant layer response under high β fusion reactor conditions.

Lee, Yeongsun (ORCID:000000034474416X)↗

DOE OSTI2024

Cooling and instabilities in colliding radiative flows with toroidal magnetic fields

ABSTRACT We report on the results of a simulation-based study of colliding magnetized plasma flows. Our set-up mimics pulsed power laboratory astrophysical experiments but, with an appropriate frame change, is relevant to astrophysical jets with internal velocity variations. We track the evolution of the interaction region where the two flows collide. Cooling via radiative losses is included in the calculation. We systematically vary plasma beta (βm) in the flows, the strength of the cooling (Λ0), and the exponent (α) of temperature dependence of the cooling function. We find that for strong magnetic fields a counter-propagating jet called a ‘spine’ is driven by pressure from shocked toroidal fields. The spines eventually become unstable and break apart. We demonstrate how formation and evolution of the spines depend on initial flow parameters and provide a simple analytical model that captures the basic features of the flow.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Monte Carlo Event Generation with Continuous Normalizing Flows

We apply continuous normalizing flows trained with the flow matching method to the problem of phase-space sampling in Monte Carlo event generation for high-energy collider physics. Focusing on lepton-pair and top-quark pair production with multiple jets, the two computationally most expensive processes at the Large Hadron Collider, we train helicity-conditioned continuous normalizing flows to remap the random numbers used in matrix element evaluation. Compared to standard methods, we achieve unweighting efficiency improvements by factors of up to 184 and 25 for the two processes at their respective highest jet number, at the cost of an increased evaluation time. When combining the advantages of continuous normalizing flows with the fast evaluation times of coupling-layer-based flows, using the RegFlow approach, we find parton-level unweighted event generation walltime gains of about a factor of 10 at the highest jet numbers. These substantial gains highlight the promise of samplers based on machine learning for next-generation collider experiments.

Bothmann, Enrico [CERN; Gottingen U.] (ORCID:00000↗