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At least 397 records · Page 22

Molten Sodium Penetration in NaSICON Electrolytes at 0.1 A cm –2

High-conductivity solid electrolytes, such as the Na superionic conductor, NaSICON, are poised to play an increasingly important role in safe, reliable battery-based energy storage, enabling advanced sodium-based batteries. Coupled demands of increased current density (≥0.1 A cm –2 ) and low-temperature (<200 °C) operation, combined with increased discharge times for long-duration storage (>12 h), challenge the limitations of solid electrolytes. Here, we explore the penetration of molten sodium into NaSICON at high current densities. Previous studies of β"-alumina proposed that Poiseuille pressure-driven cracking (mode I) and recombination of ions and electrons within the solid electrolyte (mode II) are the two main mechanisms for Na penetration, but a comprehensive study of Na penetration in NaSICON is necessary, particularly at high current density. To further understand these modes, this work employs unidirectional galvanostatic testing of Na|NaSICON|Na symmetric cells at 0.1 A cm –2 over 23 h at 110 °C. Further, while galvanostatic testing shows a relatively constant yet increasingly noisy voltage profile, electrochemical impedance spectroscopy (EIS) reveals a significant decrease in cell impedance correlated with significant sodium penetration, as observed in scanning electron microscopy (SEM). Further SEM analysis of sodium accumulation within NaSICON suggests that mode II failure may be far more prevalent than previously considered. Further, these findings suggest that total (dis)charge density (mAh cm –2 ), as opposed to current density (mA cm –2 ), may be a more critical parameter when examining solid electrolyte failure, highlighting the challenge of achieving long discharge times in batteries using solid electrolytes. Together, these results provide a better understanding of the limitations of NaSICON solid electrolytes under high current and emphasize the need for improved electrode–electrolyte interfaces.

25 ENERGY STORAGE↗

(CrMnCoNiZn) 3 O 4 @PPy core-shell nanocomposite with excellent electrochemical performance as lithium-ion battery anode

High entropy oxides (HEOs) have an excellent potential for use as electrode materials in lithium-ion batteries (LIBs) due to their high theoretical specific capacity. In this work, spinel-structured (CrMnCoNiZn) 3 O 4 HEO nanoparticles with five elements in equal molar ratio is first generated by solution combustion method. (CrMnCoNiZn) 3 O 4 @polypyrrole (PPy) nanocomposites are prepared by in-situ polymerization method. As an anode for lithium-ion batteries, the electrochemical performance of the (CrMnCoNiZn) 3 O 4 @PPy composite outperforms that of (CrMnCoNiZn) 3 O 4 nanoparticles. The capacity is 802 mAh/g after 100 cycles at a current density of 100 mA/g, 416 mAh/g after 1000 cycles at a high current density of 1 A/g, and 360 mAh/g rate capacity at 2 A/g. The excellent electrochemical performance of the composites is mainly due to the fact that the conductive and flexible PPy is encapsulated on the high-entropy oxides, which can alleviate the volume change triggered by extraction-insertion of lithium ions process, as well as enhance the electrical conductivity and reduce the occurrence of some side reactions. Finally, this method of compositing materials can also be used in other HEOs and conductive polymers, providing a new idea to enhance the electrochemical properties of HEOs.

25 ENERGY STORAGE↗

Copper Dendrites and Surface Engineering for Enhanced CO2 Reduction Research Report Paper

The electrocatalytic reduction of CO 2 (CO 2 R) into hydrocarbon fuels, such as ethylene and ethanol, provides an attractive pathway towards closing the industrial carbon cycle and producing chemicals using renewable electricity. Existing CO 2 R technologies can exhibit C 2+ product selectivity above 74% and operating current densities over 1.3 A/cm 2 , but none can achieve both simultaneously, limiting the commercial viability and scalability of this technology. Low CO 2 concentrations at the catalyst surface and competing side reactions such as the hydrogen evolution reaction (HER) inhibit C 2+ faradaic efficiencies and operational current densities. Additionally, the use of high surface area cathode geometries to increase operational current densities is under-investigated. In this work, we electrodeposit a macroporous copper dendrite film to form high surface area cathodes. These structures are then coated with a combination of hydrophobic/hydrophilic ionomers to achieve high electrochemically active surface areas (ECSA), form regions of intrinsic porosity, and maximize catalytic availability of CO 2 . Using these techniques, we hope to maximize C 2+ faradaic efficiencies (FE) and geometric partial current densities. The treated cathode compound macrostructure (~10μm-sized pores, and ~μm-long dendrites) and concomitant surface area allows increased geometric current densities while the ionomer coating simultaneously inhibits HER and increases hydrogen availability to improve C 2+ selectivity. Our results show that careful engineering of the catalyst-electrolyte interface can enhance CO 2 reduction product selectivity and efficiency.

10 SYNTHETIC FUELS↗

Asymmetric ether solvents for high-rate lithium metal batteries

Recent electrolyte solvent design based on weakening lithium-ion solvation have shown promise in enhancing cycling performance of Li-metal batteries. However, they often face slow redox kinetics and poor cycling reversibility at high rate. Here we report using asymmetric solvent molecules substantially accelerates Li redox kinetics. Asymmetric ethers (1-ethoxy-2-methoxyethane, 1-methoxy-2-propoxyethane) showed higher exchange current densities and enhanced high-rate Li 0 plating/stripping reversibility compared to symmetric ethers. Adjusting fluorination levels further improved oxidative stability and Li 0 reversibility. The asymmetric 1-(2,2,2-trifluoro)-ethoxy-2-methoxyethane, with 2 M lithium bis(fluorosulfonyl)imide, exhibited high exchange current density, oxidative stability, compact solid–electrolyte interphase (~10 nm). This electrolyte exhibited superior performance among state-of-the-art electrolytes, enabling over 220 cycles in high-rate Li (50 μm)||LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811, 4.9 mAh cm −2 ) cells and for the first time over 600 cycles in anode-free Cu | |Ni95 pouch cells (200 mAh) under electric vertical take-off and landing cycling protocols. Our findings on asymmetric molecular design strategy points to a new pathway towards achieving fast redox kinetics for high-power Li-metal batteries.

batteries↗

High-Speed Nonpolar InGaN/GaN Superluminescent Diode With 2.5 GHz Modulation Bandwidth

We demonstrate a superluminescent diode fabricated on a nonpolar m-plane GaN substrate by employing a linearly tapered waveguide design. A high electrical -3dB modulation bandwidth ( f\n 3dB \n) of 2.5 GHz at a current density of 30 kA/cm\n 2 \n is achieved. The high modulation bandwidth is attributed to the shorter carrier recombination lifetime, the linear gain curve in the nonpolar m-plane quantum wells, and the ability to operate at high current densities while effectively suppressing lasing. We derive a general expression for the -3dB bandwidth as a function of current density for SLDs using a similar approach to that for laser diodes. The -3dB bandwidth of a nonpolar superluminescent diode increases exponentially with current density. The experimental results are consistent with the derived expression for f\n 3dB \n vs. current density.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

SPARC 3D Field Physics and Support of the Non-Axisymmetric Coil Assessment

Commonwealth Fusion Systems (CFS) is deploying SPARC, a net-energy tokamak, by 2025. A notable challenge facing all tokamak approaches to fusion energy production is maintaining a stable plasma and thereby steady energy production. “Disruptions” to plasma operation are often encountered in devices when they operate at high normalized pressure, high normalized density, or high normalized current. SPARC is unique in that it is expected to demonstrate Q>=2 in a plasma with low normalized pressure and density, but with a more modest current limit buffer sufficient to avoid disruptions. Due to both the high normalized current and high magnetic field of the SPARC design, it is expected to decrease its relative resilience to instabilities driven by non-axisymmetry in the externally applied magnetic field, termed ‘error fields’. To prevent error field driven instabilities, a primary line of defense is strict engineering tolerances in magnet fabrication and installation. A secondary line of defense is a purpose-built set of magnetic coils to correct these errors, termed error field correction coils (EFCCs). The overarching goals of this INFUSE project were to evaluate the effectiveness of the EFCCs in the SPARC design and provide guidance as to how to improve this effectiveness.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Chiral Effective Field Theory and the High-Density Nuclear Equation of State

Born in the aftermath of core-collapse supernovae, neutron stars contain matter under extraordinary conditions of density and temperature that are difficult to reproduce in the laboratory. In recent years, neutron star observations have begun to yield novel insights into the nature of strongly interacting matter in the high-density regime where current theoretical models are challenged. At the same time, chiral effective field theory has developed into a powerful framework to study nuclear matter properties with quantified uncertainties in the moderate-density regime for modeling neutron stars. In this article, we review recent developments in chiral effective field theory and focus on many-body perturbation theory as a computationally efficient tool for calculating the properties of hot and dense nuclear matter. We also demonstrate how effective field theory enables statistically meaningful comparisons among nuclear theory predictions, nuclear experiments, and observational constraints on the nuclear equation of state.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Synergizing superwetting and architected electrodes for high-rate water splitting

Water splitting is one of the most promising technologies for generating green hydrogen. To meet industrial demand, it is essential to boost the operation current density to industrial levels, typically in the hundreds of mA cm -2 . However, operating at these high current densities presents significant challenges, with bubble formation being one of the most critical issues. Efficient bubble management is crucial as it directly impacts the performance and stability of the water splitting process. Superwetting electrodes, which can enhance aerophobicity, are particularly favorable for facilitating bubble detachment and transport. By reducing bubble contact time and minimizing the size of detached bubbles, these electrodes help prevent blockage and maintain high catalytic efficiency. Here, in this review, we aim to provide an overview of recent advancements in tackling bubble-related issues through the design and implementation of superwetting electrodes, including surface modification techniques and structural optimizations. We will also share our insights into the principles and mechanisms behind the design of superwetting electrodes, highlighting the key factors that influence their performance. Our review aims to guide future research directions and provides a solid foundation for developing more efficient and durable superwetting electrodes for high-rate water splitting.

36 MATERIALS SCIENCE↗

Electrochemical conversion of coal-derived CO 2 into fuels and chemicals using a modified PEM electrolyzer. Final report

Opus 12 is developing an electrochemical process to convert CO 2 into chemicals and fuels. Using only CO 2 , water, and electricity as inputs, the electrochemical reduction of CO 2 could form the basis of an artificial carbon cycle that replaces a wide range of products that are currently derived from fossil fuel resources. We have developed a prototype that demonstrates high selectivity and current density for CO 2 conversion to CO, which can be used to make high-value products including methanol, acetic acid, polymers, and pharmaceuticals.

01 COAL, LIGNITE, AND PEAT↗

Two-temperature effects in Hall-MHD simulations of the HIT-SI experiment

A two-temperature Hall-magnetohydrodynamic (Hall-MHD) model, which evolves the electron and ion temperatures separately, is implemented in the PSI-Tet 3D MHD code and used to model plasma dynamics in the Helicity Injected Torus–Steady Inductive (HIT-SI) experiment. The two-temperature model is utilized for HIT-SI simulations in both the PSI-Tet and NIMROD codes at a number of different injector frequencies in the 14.5–68.5 kHz range. At all frequencies, the NIMROD two-temperature model results in increased toroidal current, lower chord-averaged density, higher average temperatures, outward radial shift of the current centroid, and axial symmetrization of the current centroid, relative to the single-temperature NIMROD simulations. The two-temperature PSI-Tet model illustrates similar trends, but at high frequency operation, it exhibits lower electron temperature, smaller toroidal current, and decreased axial symmetrization with respect to the single-temperature PSI-Tet model. With all models, average temperatures and toroidal currents increase with the injector frequency. Power balance and heat fluxes to the wall are calculated for the two-temperature PSI-Tet model and illustrate considerable viscous and compressive heating, particularly at high injector frequency. Parameter scans are also presented for artificial diffusivity, wall temperature, and density. Both artificial diffusivity and the density boundary condition significantly modify the plasma density profiles, leading to larger average temperatures, toroidal current, and relative density fluctuations at low densities. As a result, a low density simulation achieves sufficiently high current gain (G > 5) to generate significant volumes of closed flux lasting 1–2 injector periods.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Non-uniform longitudinal current density induced power saturation in GaAs-based high power diode lasers

The output power of modern 975 nm GaAs-based broad area diode lasers is limited by increasing carrier and photon losses at high bias. Here, we use experiment and one-dimensional calculations on these devices to reveal that higher current densities (and hence higher local recombination rates and higher losses) arise near the front facet due to spatial hole burning and that the non-uniformity is strongly affected by laser geometry, which is more severe for longer resonators and less severe for higher front facet reflectivity. Specifically, we use devices with a segmented p-contact to directly measure the current distribution along the resonator and compare this with laser simulation. Devices with a 6 mm resonator show 29% more current at the front than back, twice as large as the 15% current non-uniformity in devices with a 3 mm resonator. In contrast, increased front facet reflectivity (20% rather than 0.8%) is shown to almost halve the current non-uniformity from 29% to 18% in devices with a 6 mm resonator and reduces power saturation. Although the magnitude of current non-uniformity in experiment and theory is broadly consistent, in experiment, an additional divergence is seen in current flow (and hence recombination rate) near the facets, and earlier power saturation occurs. Finally, we discuss the possible saturation mechanisms that are not included in the simulation.

47 OTHER INSTRUMENTATION↗

Electrochemical recovery of Gd into liquid Bi in molten LiCl-KCl-GdCl 3

The electrochemical recovery of Gd into liquid Bi electrodes was investigated in molten LiCl-KCl-GdCl 3 electrolyte at 773–973 K using constant currents of 10–150 mA cm −2 . High round-trip coulombic efficiency (>97 %) was demonstrated for deposition and removal of Gd into and from liquid Bi at all temperatures, confirming chemically reversible electrode reactions towards high recovery yield of Gd using liquid Bi. Furthermore, the overpotential associated with deposition of Gd into the liquid Bi electrode gradually increased with current density and decreased with temperature. At the lowest temperature of 773 K, a steep increase in overpotential was evident at high current densities due to slower mass transport and low solubility of Gd in liquid Bi (0.5 at.% Gd). Based on the impedance spectra of Bi electrodes at 773–973 K, the exchange current density was estimated to be 110–220 mA cm −2 , indicating facile charge transfer at the liquid electrode-electrolyte interface. Post-mortem characterization of Bi cathodes after electrolysis at 873 K indicated the formation of a solid GdBi(s) compound layer at the Bi electrode surface. Chemical analysis of Bi cathodes at various deposited Gd compositions resulted in Faradaic efficiencies of ∼75–84 %, promising a high recovery yield of Gd from molten salts using a strongly-interacting liquid Bi electrode.

36 - MATERIALS SCIENCE↗

Optimized Tandem Catalyst Patterning for CO 2 Reduction Flow Reactors

Tandem catalysis involves two or more catalysts arranged in proximity within a single reaction vessel, with the aim of synergistically aligning the catalysts’ reaction pathways to maximize overall system performance. This study presents a proof of concept showing the integration of continuum transport modeling with design optimization in a simplified two-dimensional flow reactor setup for electrochemical CO 2 reduction. Ag catalysts provide the CO 2 ⟶ CO reaction capability, and Cu catalysts provide the CO ⟶ high-value products reaction capability. Given a set of input parameters, the optimization algorithm uses adjoint methods to modify the Ag/Cu surface patterning in order to maximize the current density toward high-value products, such as ethylene. The optimized designs yield significant performance enhancement especially at more negative applied voltages (i.e., stronger surface reactions) and for larger numbers of patterning sections. For an applied voltage of −1.7 V vs. SHE, the 12-section optimized design increases the current density toward ethylene by up to 65% compared to the unoptimized 2-section design. For the optimized cases, observed differences in the production and consumption of CO (the key intermediate species) and minimized zones of low CO reactant surface concentration on Cu sections explain the improved reactor performance.

CO2 reduction↗

An all-oxide electrolysis cells for syngas production with tunable H 2 /CO yield via co-electrolysis of H 2 O and CO 2

High-rate production of syngas with tunable H 2 /CO and coke-free operation is achieved in a solid-oxide electrolysis cell (SOEC). Prior to operation, controlled pre-reduction of La 0.7 Sr 0.3 Fe 0.9 Ni 0.1 O 3-δ (LSFNi) cathode is used to trigger the in-situ exsolution of Ni-Fe alloy nanoparticles with an average size of ~45 nm uniformly distributed and socketed on LSFNi backbone, enabling efficient co-electrolysis of H 2 O and CO 2 to H 2 and CO. At 1.5 V, the current density reaches ~1.0 A cm-2 at 750 °C and ~2.4 A cm -2 at 850 °C with near 100% Faradaic Efficiency. We demonstrate the feasibility of tuning the output H 2 /CO ratio by nearly two orders of magnitude (from ~0.1 to ~7) by manipulating H 2 O/CO 2 ratio of feed gas, operating temperature, and current density. Finally, stable operation for >100 h is obtained without evidence of carbon deposition, although high current density operation leads to observable deterioration of anode/electrolyte interface due to the rapid oxygen evolution.

25 ENERGY STORAGE↗

Rational solvent molecule tuning for high-performance lithium metal battery electrolytes

Electrolyte engineering improved cycling of Li metal batteries and anode-free cells at low current densities; however, high-rate capability and tuning of ionic conduction in electrolytes are desirable yet less-studied. In this study, we design and synthesize a family of fluorinated-1,2-diethoxyethanes as electrolyte solvents. The position and amount of F atoms functionalized on 1,2-diethoxyethane were found to greatly affect electrolyte performance. Partially fluorinated, locally polar –CHF 2 is identified as the optimal group rather than fully fluorinated –CF 3 in common designs. Paired with 1.2 M lithium bis(fluorosulfonyl)imide, these developed single-salt-single-solvent electrolytes simultaneously enable high conductivity, low and stable overpotential, >99.5% Li||Cu half-cell efficiency (up to 99.9%, ±0.1% fluctuation) and fast activation (Li efficiency >99.3% within two cycles). Combined with high-voltage stability, these electrolytes achieve roughly 270 cycles in 50-μm-thin Li||high-loading-NMC811 full batteries and >140 cycles in fast-cycling Cu||microparticle-LiFePO 4 industrial pouch cells under realistic testing conditions. The correlation of Li + –solvent coordination, solvation environments and battery performance is investigated to understand structure–property relationships.

25 ENERGY STORAGE↗

Giant Domain Wall Conductivity in Self‐Assembled BiFeO 3 Nanocrystals

Abstract Ever‐increasing demand on electronic devices with ultrahigh‐density non‐volatile data storage has attracted great interest in novel ferroelectric memories based on conductive ferroelectric domain walls. Embedded in an insulating material, ferroelectric domain walls have the capability of being (re)created, displaced, erased, and altered in their spatial configurations and electronic characteristics. However, the domain wall conductivities are in most cases not yet sufficiently high to ensure the current density required to drive read‐out circuits operating at high speeds. In this work, a giant domain wall current (>10 µA) of a single charged domain wall is obtained through conductive atomic force microscopy with a bias field of 4 V. This is achieved in self‐assembled BiFeO 3 nanocrystals grown by sol‐gel method on Nb‐doped SrTiO 3 substrates. Local configurations of domains and domain wall types are studied using vector piezoresponse force microscopy and high‐resolution transmission electronic microscopy. The enhancement of the wall current is shown to be due to the formation of conducting pathways of charged defects accumulated along domain walls and traversing the nanocrystals. The diverse domain walls can be manipulated by electric field in a perpendicular architecture. The perpendicular array structure of BiFeO 3 nanocrystals should have great potentials for developing perpendicular nanoelectronic prototypes.

Liu, Lisha↗

Amorphizing noble metal chalcogenide catalysts at the single-layer limit towards hydrogen production

Rational design of noble metal catalysts with the potential to leverage efficiency is vital for industrial applications. Such an ultimate atom-utilization efficiency can be achieved when all noble metal atoms exclusively contribute to catalysis. In this work, we demonstrate the fabrication of a wafer-size amorphous PtSex film on a SiO 2 substate via a low-temperature amorphization strategy, which offers single-atom-layer Pt catalysts with high atom-utilization efficiency (~26 wt%). This amorphous PtSex (1.2 < x < 1.3) behaves as a fully activated surface, accessible to catalytic reactions, and features a nearly 100% current density relative to a pure Pt surface and reliable production of sustained high-flux hydrogen over a 2 inch wafer as a proof-of-concept. Furthermore, an electrolyser is demonstrated to generate a high current density of 1,000 mA cm –2 . Such an amorphization strategy is potentially extendable to other noble metals, including the Pd, Ir, Os, Rh and Ru elements, demonstrating the universality of single-atom-layer catalysts.

36 MATERIALS SCIENCE↗

Advanced silver sheathed 2212/Ag wire for high field magnets

Commercial High Temperature Superconductors (HTS) are all tape shaped (widths > 10 times thickness), because achieving useful current densities required them to be processed into this form, even though this also makes it more problematic to use them in some important coil types. Our product is based on 2212 (Bi2Sr2CaCu2O8) and it is the only HTS that can be processed into high current density wire forms that are similar to proven low temperature superconductors (LTS), while surpassing them in field generating and operating temperature capability. Required now are higher current density, lower cost and longer length 2212 wires to enable broad utilization where HTS tape usage is problematic. In Phase II we developed vital cost-lowering process technology elements and we test-processed longer wires with the standard commercial design as baseline and benchmark for our lower cost, higher quality and longer piece length wire advances. By initial application of Jc-boosting wire features, these wires exhibited significant performance increases. This Phase IIA program has now developed and qualified these technologies for lower cost, higher quality and longer piece length manufacturing in combination with current density-boosting wire features, paving the way to manufacturing capability that is essential for cost-effective commercial utilization of 2212 wire. Technical areas included automated, high uniformity powder packing, advanced drawing, annealing, lubricant cleaning and filament bundling, followed by integration of higher current density wire features and process variations.

17 WIND ENERGY↗