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At least 145 records · Page 8

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DOE OSTI2020

An epoxy-reinforced ceramic sheet as a durable solid electrolyte for solid state Na-ion batteries

In a conventional Na-ion battery system using liquid electrolyte, there are critical safety issues due to the instability of the liquid electrolyte. Na 3 Zr 2 Si 2 PO 12 (NASICON) solid electrolyte is a material that is sufficient to replace a liquid electrolyte as it has high ionic conductivity and thermal and electrochemical stability. However, as there is a large interfacial resistance in the NASICON solid electrolyte powder, even when used in combination with a polymer electrolyte, the advantageous effects of ceramics are not easily exhibited. In this study, we propose a top-down method of combining a polymer with a ceramic in which an ion transport channel is previously formed. In this method, a NASICON solid electrolyte is partially sintered to form ion transport channels. Then the NASICON solid electrolyte pores are filled with an epoxy polymer to increase the strength of the epoxy-NASICON composite electrolyte. This method demonstrates the possibility of our composite electrolyte being used as a thin and strong film. As a result of our methods, the ionic conductivity and thermal and electrochemical stability of NASICON were maintained, while the physical strength was enhanced by approximately 2 times. In addition, a capacity of 120 mA h g -1 and stability of 20 cycles were confirmed in a half cell with a Na 3 V 2 (PO 4 ) 3 cathode and Na metal. This method proposes a new direction for research regarding composite electrolytes created using an oxide-based solid electrolyte.

25 ENERGY STORAGE↗

DOE OSTI2022

Evidence for pressure induced unconventional quantum criticality in the coupled spin ladder antiferromagnet C 9 H 18 N 2 CuBr 4

Quantum phase transitions in quantum matter occur at zero temperature between distinct ground states by tuning a nonthermal control parameter. Often, they can be accurately described within the Landau theory of phase transitions, similarly to conventional thermal phase transitions. However, this picture can break down under certain circumstances. Here, we present a comprehensive study of the effect of hydrostatic pressure on the magnetic structure and spin dynamics of the spin-1/2 ladder compound C 9 H 18 N 2 CuBr 4 . Single-crystal heat capacity and neutron diffraction measurements reveal that the Néel-ordered phase breaks down beyond a critical pressure of Pc~1.0 GPa through a continuous quantum phase transition. Estimates of the critical exponents suggest that this transition may fall outside the traditional Landau paradigm. The inelastic neutron scattering spectra at 1.3 GPa are characterized by two well-separated gapped modes, including one continuum-like and another resolution-limited excitation in distinct scattering channels, which further indicates an exotic quantum-disordered phase above Pc.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Fabrication of a composite anion exchange membrane with aligned ion channels for a high-performance non-aqueous vanadium redox flow battery

Fabrication of high-conductivity ion exchange membranes (IEMs) is crucial to improve the performance of non-aqueous vanadium redox flow batteries (NAVRFBs). In the present work, anion exchange membranes with high-conductivity were fabricated by aligning ion channels of the polymer electrolyte impregnated in porous polytetrafluoroethylene (PTFE) under electric fields. It was observed that the ion channels of the polymer electrolyte were uniformly orientated in the atomic-force microscopy image. Its morphological change could minimize detouring of the transport of BF 4 - ions. The results showed through-plane conductivity was improved from 12.7 to 33.1 mS cm -1 . The dimensional properties of the fabricated membranes were also enhanced compared with its cast membrane owing to the reinforcing effect of the substrate. Especially, the NAVRFB assembled with the optimized membrane showed increased capacities, with a 97% coulombic efficiency and 70% energy efficiency at 80 mA cm -2 . Furthermore, the optimized membrane made it possible to operate the NAVRFB at 120 mA cm -2 . Its operating current density was 120 times higher than that of a frequently used AHA membrane for RFBs.

25 ENERGY STORAGE↗

DOE OSTI2020

Conjugate Heat Transfer Analysis of the Supercritical CO2 Based Counter Flow Compact 3D Heat Exchangers

Compact heat exchangers using supercritical fluids such as CO2 are preferred due to their high heat transfer capacity and smaller footprint. Three-dimensional conjugate forced convection heat transfer analysis was performed on several shell-and-tube counter-flow microchannel heat exchangers. Numerical simulations were conducted to test effect of change in mass flow rate, hydraulic diameter and various cross sections on the heat transfer. Increasing mass flow rate improved heat transfer up to a maximum value and then decreased downstream with increasing turbulence. Maximum heat transfer was obtained for the micro channel with the smallest hydraulic diameter. Amongst the cross sections analyzed (circular, square, circular with radial ribs, and square with radial ribs), the most uniform distribution of temperature and maximum heat transfer were obtained for circular cross section with radial ribs. An optimally efficient operation of such a heat exchanger can be attained by considering these factors during multi-objective constrained optimization of geometric parameters and requirements for additive manufacturing of such compact heat exchangers.

Chitale, Janhavi↗

DOE OSTI2020

Conjugate Heat Transfer Analysis of the Supercritical CO2 Based Counter Flow Compact 3D Heat Exchangers

Chitale, Janhavi↗

DOE OSTI2022

Bilayer hybrid graphite anodes via freeze tape casting for extreme fast charging applications

Extreme fast charging (XFC) of lithium-ion batteries is critical for continuous market adoption of electric vehicles. However, mass transport limitations and sluggish kinetics lead to lithium plating in graphite anodes under fast charging conditions. One approach to address the mass transport limitation in graphite is to design low-tortuosity electrodes to enhance ionic transport. In this study, a bilayer hybrid structured electrode with directionally aligned channels was developed via freeze tape casting, which enables faster lithium ion diffusion through the graphite electrode. A scalable roll-to-roll process was designed in which slurry can be cast on any substrates for simple processing. Additionally, electrochemical impedance spectroscopy measurements indicated that the bilayer hybrid coating had both low tortuosity and short diffusion pathways, enabling XFC charging. Rate testing for the bilayer hybrid electrode indicated superior performance over the other coatings, exhibiting a ~20% improvement in the charge capacity compared with the conventional coating at 5C and 10 min total charging time. The bilayer hybrid electrode also demonstrated a 10% improvement in capacity retention compared with the conventional electrode after 1000 cycles at XFC conditions. This study demonstrates freeze tape casting as a scalable way to fabricate low-tortuosity electrodes for XFC applications.

25 ENERGY STORAGE↗

DOE OSTI2020

Solution-Based, Anion-Doping of Li 4 Ti 5 O 12 Nanoflowers for Lithium-Ion Battery Applications

Solution–based, anionic doping represents a convenient strategy with which to improve upon the conductivity of candidate anode materials such as Li 4 Ti 5 O 12 (LTO). As such, novel synthetic hydrothermally–inspired protocols have primarily been devised herein, aimed at the large–scale production of unique halogen–doped, micron–scale, three–dimensional, hierarchical LTO flower–like motifs. Although fluorine (F) doping has been explored, the use of chlorine (Cl) dopants is the primary focus here. Several experimental variables, such as dopant amount, lithium hydroxide concentration, and titanium butoxide purity, were probed and perfected. Furthermore, the Cl doping process did not damage the intrinsic LTO morphology. The analysis, based on interpreting a compilation of SEM, XRD, XPS, and TEM–EDS results, was used to determine an optimized dopant concentration of Cl. Electrochemical tests demonstrated an increased capacity via cycling of 12 % for a Cl–doped sample as compared with pristine LTO. Moreover, the Cl–doped LTO sample described in this study exhibited the highest discharge capacity yet reported at an observed rate of 2C for this material at 143mAh g –1 . Overall, these data suggest that the Cl dopant likely enhances not only the ion transport capabilities, but also the overall electrical conductivity of our as–prepared structures. Furthermore, to help explain these favorable findings, theoretical DFT calculations were used to postulate that the electronic conductivity and Li diffusion were likely improved by the presence of increased Ti 3+ ion concentration coupled with widening of the Li migration channel.

25 ENERGY STORAGE↗

DOE OSTI2020

Detachment in Fusion Plasmas with Symmetry Breaking Magnetic Perturbation Fields

Power exhaust from the bulk plasma is significantly altered by symmetry breaking magnetic perturbation fields, because these create direct connections (perturbed field lines) from the confined high temperature plasma to solid surfaces. Additionally, the same amount of power is distributed among those new exhaust channels as for a symmetric magnetic configuration, which reduces the local upstream heat flux flowing down the perturbed field lines, thereby making access to detachment easier (i.e., at lower upstream density) for the divertor plasma near the location corresponding to the symmetric magnetic separatrix. However, the divertor plasma regions with connection to the bulk plasma are extended nonaxisymmetrically further outside, where significant heat loads occur, unlike in the symmetric configuration. The temperature remains high at those locations, which reduces the divertor plasma dissipation capacity, making the mitigation of heat loads more difficult to achieve.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

A User Guide to PARET/ANL

PARET was originally created in 1969 at what is now Idaho National Laboratory (INL), to analyze reactivity insertion events in research and test reactor cores cooled by light or heavy water, with fuel composed of either plates or pins. The use of PARET is also appropriate for fuel assemblies with curved fuel plates when their radii of curvatures are large with respect to the fuel plate thickness. The PARET/ANL version of the code has been developed at Argonne National Laboratory (ANL) under the sponsorship of the U.S. Department of Energy/NNSA since the inception of the Reactor Conversion Program. Since Reduced Enrichment for Research and Test Reactors (RERTR) began in 1978, PARET/ANL has been benchmarked to experimental data including SPERT testing, and used to determine the expected transient behavior of a large number of reactors regardless of enrichment both inside and outside the Reactor Conversion Program. This document provides the pertinent information for the use of PARET/ANL Version 7.6. PARET/ANL models the various fueled regions of a reactor core as channels. Each of these channels consists of a single flat fuel plate/pin (including cladding and, optionally, a gap) with water coolant on each side. In slab geometry the coolant channels for a given fuel plate are of identical dimensions (mirror symmetry), but they can be of different thickness in each channel. There can be many channels, but each channel is independent and coupled only through reactivity feedback effects to the whole core. The time-dependent differential equations that represent the system are replaced by an equivalent set of finite-difference equations in space and time, which are integrated numerically. PARET/ANL uses fundamentally the same numerical scheme as RELAP5 for the time-integration of the point-kinetics equations. The one-dimensional thermal-hydraulic model includes temperature-dependent thermal properties of the solid materials, such as heat capacity and thermal conductivity, as well as the transient heat production and heat transfer from the fuel meat to the coolant. Temperature- and pressure-dependent thermal properties of the coolant such as enthalpy, density, thermal conductivity, and viscosity are also used in determining parameters such as friction factors and heat transfer coefficients. The code first determines the steady-state solution for the initial state. Then the solution of the transient is obtained by integration in time and space. Multiple heat transfer, DNB and flow instability correlations are available. The code was originally developed to model reactors cooled by an open loop, which was adequate for rapid transients in pool-type cores. An external loop model appropriate for Miniature Neutron Source Reactors (MNSR’s) was also added to PARET/ANL to model natural circulation within the vessel, heat transfer from the vessel to pool and heat loss by evaporation from the pool. PARET/ANL also contains models for decay heat after shutdown, control rod reactivity versus time or position, time-dependent pump flow, and loss-of-flow event with flow reversal as well as logic for trips on period, power, and flow. Feedback reactivity effects from coolant density changes and temperature changes are represented by tables. Feedback reactivity from fuel heat-up (Doppler Effect) is represented by a four-term polynomial in powers of fuel temperature. Photo-neutrons produced in beryllium or in heavy water may be included in the point-kinetics equations by using additional delayed neutron groups.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Heat transfer model for moving packed-bed particle-to-sCO 2 heat exchangers integrated with metal foams

Particle-to-supercritical carbon dioxide (sCO 2 ) heat exchangers (HXs) play a vital role in coupling heat transfer fluid (HTF) from high-temperature thermal receivers to power cycle working fluids (WF). Heat transfer enhancement is essential for adopting particle-based moving packed-bed heat exchangers (MPBHXs) in next-generation thermal energy storage (TES) systems, as MPBHXs usually exhibit low particle bed-to-wall heat transfer coefficients. High-porosity metal foams have shown their effectiveness in heat transfer enhancement. Here, this work presents a continuum heat transfer model to demonstrate the heat transfer enhancement in MPBHXs when the particle bed channel is filled with high porosity metal foams compared to open channel MPBHXs. The presence of metal foams increases the effective thermal conductivity in the particle channel and enhances the interstitial heat transfer coefficient between the moving particle bed and the stationary metal foams. The present model considers coupled two-dimensional (2D) heat transfer in the particle channel with metal foams and 1D heat transfer in the sCO 2 channel and the dividing wall. The temperature profiles for the particle bed, metal foam, dividing wall, and sCO 2 stream, as well as the local heat flux profiles between those, are studied in detail for various foam porosities, from which the particle bed-to-wall heat transfer coefficient, overall heat transfer coefficient, and total heat transfer rate for the MPBHX are determined. The effects of major MPBHX design and operating parameters on the particle bed-to-wall heat transfer coefficient and overall heat exchange capacity are thoroughly examined; thus, the MPBHX performance improvement with metal foams is quantified for each case. The present heat transfer model can provide valuable insights into the metal-foam MPBHX design and optimization, scale-up, and operating parameters selection.

42 ENGINEERING↗

DOE OSTI2022

Broadband polarization-entangled source for C+L-band flex-grid quantum networks

The rising demand for transmission capacity in optical networks has motivated steady interest in expansion beyond the standard C-band (1530–1565 nm) into the adjacent L-band (1565–1625 nm) for an approximate doubling of capacity in a single stroke. However, in the context of quantum networking, the L-band has yet to be fully leveraged with the suite of advanced tools for characterization and management available from classical lightwave communications. In this work, we demonstrate an ultrabroadband two-photon source integrating both C- and L-band wavelength-selective switches for complete control of spectral routing and allocation across 7.5 THz in a single setup. Polarization state tomography of all 150 pairs of 25-GHz-wide channels reveals an average fidelity of 0.98 and total distillable entanglement greater than 181 kebits/s. This source is explicitly designed for flex-grid optical networks and can facilitate optimal utilization of entanglement resources across the full C+L-band.

42 ENGINEERING↗

DOE OSTI2020

A micromirror array with annular partitioning for high-speed random-access axial focusing

Dynamic axial focusing functionality has recently experienced widespread incorporation in microscopy, augmented/virtual reality (AR/VR), adaptive optics and material processing. However, the limitations of existing varifocal tools continue to beset the performance capabilities and operating overhead of the optical systems that mobilize such functionality. The varifocal tools that are the least burdensome to operate (e.g. liquid crystal, elastomeric or optofluidic lenses) suffer from low (≈100 Hz) refresh rates. Conversely, the fastest devices sacrifice either critical capabilities such as their dwelling capacity (e.g. acoustic gradient lenses or monolithic micromechanical mirrors) or low operating overhead (e.g. deformable mirrors). Here, we present a general-purpose random-access axial focusing device that bridges these previously conflicting features of high speed, dwelling capacity and lightweight drive by employing low-rigidity micromirrors that exploit the robustness of defocusing phase profiles. Geometrically, the device consists of an 8.2 mm diameter array of piston-motion and 48-μm-pitch micromirror pixels that provide 2π phase shifting for wavelengths shorter than 1100 nm with 10–90% settling in 64.8 μs (i.e., 15.44 kHz refresh rate). The pixels are electrically partitioned into 32 rings for a driving scheme that enables phase-wrapped operation with circular symmetry and requires <30 V per channel. Optical experiments demonstrated the array’s wide focusing range with a measured ability to target 29 distinct resolvable depth planes. Overall, the features of the proposed array offer the potential for compact, straightforward methods of tackling bottlenecked applications, including high-throughput single-cell targeting in neurobiology and the delivery of dense 3D visual information in AR/VR.

42 ENGINEERING↗

DOE OSTI2022

Deploying Taller Turbines in Complex Terrain: A Hill Flow Study (HilFlowS) Perspective

Terrain-induced flow acceleration is presented for the summertime, peak power season at Lawrence Livermore National Laboratory’s Site 300 for the Hill Flow Study (HilFlowS). HilFlowS, designed as an adjunct field campaign to the Department of Energy’s Second Wind Forecasting Improvement Project (WFIP2), provides wind profile observations at a second location in complex terrain for validating numerical atmospheric model simulations and for better understanding flow behavior over hills for wind power generation. One unique feature of HilFlowS was the inclusion of an undergraduate university student who helped plan and execute the experiment as well as analyze wind data from two remote sensing laser detection and ranging (lidar) instruments deployed along parallel ridgelines. HilFlowS examines the trend of building higher into the atmosphere for the purpose of increasing wind turbine power production and evaluates the wind resource in the Altamont Pass Region of Northern California for a set of wind turbines of differing hub-heights and rotor-disk diameters found in the area. The wind profiles show strongly channeled onshore flow above both hills, enhanced by strong subsidence aloft, which produces a wind maximum (Umax) around z = 10 m and strong negative shear throughout all of the evaluated rotor-disks for much of the summer wind season. Under these conditions, shear becomes more negative with increasing hub-height and increasing rotor-disk size. Rotor-disk equivalent wind speed (Uequiv), a measure of the average wind speed across the entire rotor-disk, is compared to hub-height, rotor length, and rated capacity factor for the set of turbines. Uequiv is most closely related to turbine hub-height and is negatively correlated given the low altitude of Umax. Based on these results, building the largest capacity, large rotor-disk wind turbine at the lowest possible hub-height appears to provide turbines in the Altamont with a fast, near-surface, onshore wind resource during the peak power season.

17 WIND ENERGY↗

DOE OSTI2025

Self-Supported Branched Poly(ethylenimine) Monoliths from Inverse Template 3D Printing for Direct Air Capture

3D-printed inverse templates are combined with ice templating to develop self-supported branched poly(ethylenimine) monoliths with regular channels of varying channel density and ordered macropores. A maximum uptake of 0.96 mmol of CO 2 /g of monolith from ambient air containing 45.5% RH is achieved from dynamic breakthrough experiments, which is a 31% increase compared to the CO 2 uptake from adsorption under dry conditions for the same duration. The breakthrough experiments show characteristics of internal mass-transfer limitations. The cyclic dynamic breakthrough experiments indicate stable operation without significant loss in CO 2 uptake across eight cycles. Moreover, the self-supported monolith shows minimal loss in adsorption capacity (7.7%) upon exposure to air containing 21% oxygen at 110 °C, in comparison to a conventional sorbent consisting of poly(ethylenimine) impregnated on Al 2 O 3 (18.9%). The monoliths exhibit good mechanical stability, contributed by elastic deformation, corresponding to up to 74% strain and lower pressure drop compared to many existing monoliths in the literature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Quantum entanglement distribution coexisting with high-rate, broadband classical optical communications over a real-world fiber connecting remote, synchronized nodes

Compatibility with existing classical network infrastructure offers a scalable path towards deploying large-scale quantum networks. Here, we demonstrate O-band polarization-encoded quantum entanglement distribution over an installed 24.4-km fiber while coexisting with a state-of-the-art fully loaded C-band classical communications line system and a picosecond-level precision L-band synchronization signal. The classical system carries two 800-Gbps channels while the remainder of the C-band is filled with amplified spontaneous emission, as is standard for such state-of-the-art communications systems. We examine the spontaneous Raman scattering spectrum generated from this broadband C-band light and offer insights into wavelength allocation for O-band quantum channels. Optimal wavelength selection and narrow filtering enable well-preserved Bell state fidelity when coexisting with 21.4-dBm aggregate launch power across the C-band suitable for 36-Tbps transmission. To the best of our knowledge, this is the first implementation of entanglement-based quantum communications between two remote nodes coexisting with independent classical communications traffic. We demonstrate coexistence of quantum entanglement with ultra-high power levels and record classical bandwidth, offering promise for real-world entanglement-based networking integrated within high-capacity communications infrastructure.

Talcott, Gina M. [Northwestern U.] (ORCID:00000002↗

DOE OSTI2020

Lithium Manganese Spinel Cathodes for Lithium-Ion Batteries

Spinel LiMn 2 O 4 , whose electrochemical activity was first reported by Professor John B. Goodenough’s group at Oxford in 1983, is an important cathode material for lithium-ion batteries, which attracts continuous academic and industrial interests. It is cheap and environmentally friendly, and has excellent rate performance with 3-dimensional (3D) Li + diffusion channels. However, it suffers from severe degradations, especially under extreme voltages and during high-temperature operations. In this review, the current understanding and future trends of the spinel cathode and its derivatives with cubic lattice symmetry (LiNi 0.5 Mn 1.5 O 4 that shows high-voltage stability, and Li-rich spinels that show reversible hybrid anion- and cation-redox activities) shall be discussed. Special attention is given to the degradation mechanisms, further development of spinel cathodes, and concepts of utilizing the cubic spinel structure to stabilize high-capacity layered cathodes and as robust framework for high-rate electrodes. Lastly, “Good spinel” surface phases like LiNi 0.5 Mn 1.5 O 4 are distinguished from “bad spinel” surface phases like Mn 3 O 4 .

25 ENERGY STORAGE↗

DOE OSTI2025

Constraining Interlayer Slipping in P2-Type Layered Oxides with Oxygen Redox by Constructing Strong Covalent Bonds

Lattice oxygen redox (LOR) in P2-type layered oxides is an effective strategy to break through the limit of energy density of conventional cathodes due to its high redox potential (>4 V vs. Na + /Na) as well as extra capacity. Nevertheless, LOR induced local structure distortion and irreversible phase transitions cause serious electrochemical performance degradation, hindering the practical applications. In this work, we propose that the generation of the OP4 phase can be replaced with the Z phase by introducing Sb element with higher ionic potential and strong covalent bonds within the TMO 6 octahedron. Z phase transition is realized by constraining interlayer slipping between adjacent TM layers compared to OP4, which reduces the strain in the layered structure, lowers the Na+ diffusion energy barrier and creates more efficient Na+ diffusion channels. Consequently, Sb-substituted oxides demonstrates excellent kinetics, rate capability (79 mAh g -1 at 1 A g -1 ) in half cell and a high energy density of 487 Wh kg -1 (on cathode) in full cell.

25 ENERGY STORAGE↗

DOE OSTI2024

Self-Assembled Bolaamphiphile-Based Organic Nanotubes as Efficient Cu(II) Ion Adsorbents

Self-assembled organic nanotubes (ONTs) have been actively examined for various applications such as chemical separations and catalysis owing to their well-defined tubular nanostructures with distinct chemical environments at the wall and internal/external surfaces. Adsorption of heavy metal ions onto ONTs plays an essential role in many of these applications, but it has rarely been assessed quantitatively. Herein, we investigated interactions between Cu 2+ and single-/quadruple-wall bolaamphiphile-based ONTs having inner carboxyl groups with different inner diameters, COOH-ONT 10nm and COOH-ONT 20nm . We first examined the effects of Cu 2+ on their nanotubular structures using SAXS, STEM, and AFM. COOH-ONT 10nm was stable in aqueous Cu 2+ solution in contrast to COOH-ONT 20nm owing to the presence of polyglycine-II-type hydrogen bonding networks within its wall. Subsequently, we studied the Cu 2+ adsorption behavior of COOH-ONT 10nm by monitoring the concentration of unbound Cu 2+ using linear sweep anodic stripping voltammetry. The Cu 2+ adsorption was quick, attributable to efficient Cu 2+ partitioning through the open ends of the ONT, followed by fast Cu 2+ diffusion in the uniform, relatively large nanochannel. More importantly, the Cu 2+ adsorption capacity and affinity of COOH-ONT 10nm were measured at different pH using the Langmuir adsorption model. The adsorption capacity was similar at the pH range examined, showing the participation of approximately 25% of the inner carboxyl groups in the adsorption. The adsorption affinity increased with pH, indicating the essential role of the deprotonated carboxyl groups in the Cu 2+ adsorption. Most interestingly, the Langmuir adsorption constant was significantly higher than those of previously reported synthetic adsorbents and planar monolayer based on carboxyl binding sites. The high Cu 2+ affinity of the ONT was attributable to the highly dense binding sites on the well-defined nanoscale concave structure of the inner channel. Furthermore, these results provide a valuable guideline to designing self-assembled nanomaterials for efficient chemical separations, detection, and catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗