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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Molecular Tuning of Ether Cosolvent Chemistry for High-Voltage Sodium-Ion Batteries

Ethers as electrolyte cosolvents in sodium-ion batteries (SIBs) provide favorable Na + solvation and interfacial properties, but their low oxidative stability limits their use in high-voltage SIBs. Herein, we address this limitation via molecular tuning of ether cosolvents for high-voltage (4.2 V) hard carbon || NaNi 0.33 Fe 0.33 Mn 0.33 O 2 full cells. Tetrahydropyran (THP) is functionalized with a nitrile group to form tetrahydropyran-4-carbonitrile (THPCN). To delineate the effect of nitrile functionalization and benchmark ether against a conventional carbonate, THP, THPCN, and diethyl carbonate (DEC) are evaluated as cosolvents with ethylene carbonate. Nitrile functionalization lowers the HOMO energy of the ether, extends the electrolyte stability window, and alters Na⁺ solvation. Spectroscopic techniques and molecular dynamics simulations reveal that THPCN exhibits predominantly aggregate-dominated solvation (95.1 %) with weakened Na + -solvent interactions, producing the most anion-rich environment relative to DEC and THP cosolvents. THPCN-modified solvation promotes the formation of highly conductive, fluorine-enriched interphases that suppress parasitic reactions. Pouch full cells with THPCN sustained ~ 600 cycles at 4.2 V, outperforming THP and DEC. Operando gas analysis reveals that THPCN reduces CO 2 generation by 45% and H 2 generation by 30% relative to THP. Furthermore, the findings demonstrate nitrile functionalization as a molecular design strategy to stabilize ethers and enable high-voltage SIBs.

25 ENERGY STORAGE↗
DOE OSTI2025

Delineating the Impact of Diluent on High-Concentration Electrolytes for Developing High-Voltage LiNi 0.5 Mn 1.5 O 4 Spinel Cathode

LiNi 0.5 Mn 1.5 O 4 (LNMO) is a high-voltage spinel cathode with low nickel content, making it an attractive candidate for next-generation lithium-ion batteries (LIBs). However, its application is limited by interfacial instability with conventional carbonate-based electrolytes at high voltages. In this work, a localized saturated electrolyte (LSE) capable of stably operating up to 4.85 V is investigated. Molecular dynamics simulations and Fourier transform infrared spectroscopy reveal that adding “non-solvating” 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether diluent in the saturated electrolyte, more PF 6 − anions are present in the first solvation shell of Li + , at the expense of solvent molecules. This tailored solvation environment promotes the formation of a robust, LiF-rich cathode-electrolyte interphase that mitigates transition metal dissolution and parasitic side reactions. The optimized LSE enables excellent cycling performance, with 95% capacity retention in Li|LNMO half-cells after 100 cycles and 94% retention in Li 4 Ti 5 O 12 |LNMO full cells after 250 cycles, even at a practically relevant LNMO cathode loading of ≈15 mg cm −2 . In conclusion, these results highlight the benefits of electrolyte engineering and solvation structure control in advancing high-voltage LIB technologies.

LNMO cathode↗
DOE OSTI2022

A Prototype High-Voltage Pulsed Power Supply for Control of the ITER Shattered Pellet Injection System Flyer Plate Valve

A high-voltage pulsed power supply (HVPPS) has been designed, prototyped, and tested for driving an eddy current actuated propellant valve for the International Thermonuclear Experimental Reactor (ITER) disruption mitigation system. The high-voltage (HV) dc supply output voltage is software programmable, and the energy storage capacitor bank can be readily reconfigured as 200, 400, 600, and 800 μ F, enabling testing and optimization of both the valve drive and valve systems. Multiple system parameters are monitored before, during, and after each firing of the valve. The system parameters are both displayed and stored for further analysis. Control of the setup, firing sequence, and data collection is automated using a LabVIEW-based control program. The programmability and reconfigurability of this system collectively provide a flexible and robust platform for system refinement and optimization. In this article, a summary of the system will be provided including operational sequences, HV switching and associated triggering methods and circuits, and results measured while firing a solid frozen pellet. Additionally, planned refinement activities toward meeting all requirements for ITER integration will be discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Unveiling the High‐Voltage Reactivity and Gas Evolution With Aluminum‐Based Chloride and Oxychloride Catholytes in Solid‐State Sodium Batteries

All-solid-state sodium batteries (ASSBs) employing halide solid electrolytes (SEs) offer a cost-effective and energy-dense alternative to conventional liquid electrolyte systems. However, their high voltage (>4 V vs. Na/Na + ) performance remains limited by interfacial instability between the cathode active material (CAM) and the SE. We present here the electrochemical and interfacial behaviors of crystalline NaAlCl 4 and amorphous sodium–aluminum–oxychloride (NACO) SEs when combined with NaNi 0.5 Mn 0.5 O 2 cathode. While oxygen incorporation in NACO enhances ionic conductivity by nearly three orders of magnitude relative to NaAlCl 4 , it does not improve high-voltage cycling stability. Cells employing NACO exhibit accelerated capacity fade, increased cell impedance growth, and intrinsic oxygen evolution above 4.5 V vs. Na 3 Sn, as revealed by operando electrochemical mass spectrometry. In contrast, the NaAlCl 4 -based cells show no detectable gas release, underscoring their superior high-voltage stability and safety. Time-of-flight secondary-ion mass spectrometry confirms the formation of Al─O and Ni/Mn─Cl species, respectively, in the SE and CAM, indicating redox-driven anion exchange that contributes to kinetic hindrance of high-voltage phase transitions. The findings establish that while oxygen incorporation enhances ionic transport, it can compromise interfacial stability, suggesting pure chloride SEs may offer a more robust and intrinsically safer pathway for developing high-energy ASSBs.

25 ENERGY STORAGE↗
DOE OSTI2024

Defect Chemistry in High‐Voltage Cathode Materials for Lithium‐Ion Batteries

High-voltage cathodes (HVCs) have emerged as a paramount role for the next-generation high-energy-density lithium-ion batteries (LIBs). However, the pursuit of HVCs comes with inherent challenges related to defective structures, which significantly impact the electrochemical performance of LIBs. The current obstacle lies in the lack of a comprehensive understanding of defects and their precise effects. This perspective aims to provide insights into defect chemistry for governing HVCs. The classifications, formation mechanisms, and evolution of defects are outlined to explore the intricate relationship between defects and electrochemical behavior. The pressing need for cutting-edge characterization techniques that comprehensively investigate defects across various temporal and spatial scales is emphasized. Building on these fundamental understandings, engineering strategies such as composition tailoring, morphology design, interface modification, and structural control to mitigate or utilize defects are thoroughly discussed for enhanced HVCs performance. Furthermore, these insights are expected to provide vital guidelines for developing high-performance HVCs for next-generation high-energy lithium-ion batteries.

cross-scale characterization↗
DOE OSTI2024

Deciphering Chemical/Electrochemical Compatibility of Li 3 InCl 6 in 5.2 V High-Voltage LiCoO 2 All-Solid-State Batteries

Large interfacial resistance is a widely recognized impediment to the advancement of high-voltage, all-solid-state batteries. However, a comprehensive understanding of the fundamental cause behind the interfacial resistance between solid electrolytes and typical layered oxide cathodes has not yet been achieved. Here, we investigated the high-voltage stability of Li 3 InCl 6 and elucidated the underlying interfacial electrochemical reactions between LiCoO 2 and Li 3 InCl 6 . Further, the pairing of Li 3 InCl 6 with LiCoO 2 exhibited a superior capacity retention of 73.6% even at 5.2 V, much higher than 28.2% charged at 4.6 V in lithium-ion batteries after 70 cycles. The enhanced high-voltage stability of ASSBs is attributed to the stable interface formed between LiCoO 2 and Li 3 InCl 6 and the reinforced surface and bulk structure stability. On the other hand, the ultrahigh voltage still causes the partial decomposition of Li 3 InCl 6 and generates interfacial compounds such as InClO and cobalt and indium chlorides/oxides.

25 ENERGY STORAGE↗
DOE OSTI2023

HERACLES: A high-voltage DC test beamline for high average current photocathodes

Here, we present commissioning results of the High ElectRon Average Current for Lifetime ExperimentS (HERACLES) beamline at Cornell University. 10 mA average beam current at 200 keV was achieved with a Cs3Sb photocathode operated with an Argon laser at 488 nm. HERACLES is intended to be a test facility to improve the robustness of photocathodes developed for high average current beam operation in conjunction with the Cornell photocathode laboratory.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Steric Effect Tuned Ion Solvation Enabling Stable Cycling of High-Voltage Lithium Metal Battery

1,2-Dimethoxyethane (DME) is a common electrolyte solvent for lithium metal batteries. Various DME-based electrolyte designs have improved long-term cyclability of high-voltage full cells. However, insufficient Coulombic efficiency at the Li anode and poor high-voltage stability remain a challenge for DME electrolytes. Here, we report a molecular design principle that utilizes a steric hindrance effect to tune the solvation structures of Li + ions. In this work, we hypothesized that by substituting the methoxy groups on DME with larger-sized ethoxy groups, the resulting 1,2-diethoxyethane (DEE) should have a weaker solvation ability and consequently more anion-rich inner solvation shells, both of which enhance interfacial stability at the cathode and anode. Experimental and computational evidence indicates such steric-effect-based design leads to an appreciable improvement in electrochemical stability of lithium bis(fluorosulfonyl)imide (LiFSI)/DEE electrolytes. Under stringent full-cell conditions of 4.8 mAh cm –2 NMC811, 50 μm thin Li, and high cutoff voltage at 4.4 V, 4 M LiFSI/DEE enabled 182 cycles until 80% capacity retention while 4 M LiFSI/DME only achieved 94 cycles. This work points out a promising path toward the molecular design of non-fluorinated ether-based electrolyte solvents for practical high-voltage Li metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Garnet solid electrolyte blended LiNi 0.6 Mn 0.2 Co 0.2 O 2 as high-voltage stable cathodes for advanced lithium-ion batteries

Ni-rich LiNi 1-x Co x/2 Mn x/2 O 2 layered materials have been widely adopted as cathodes for current electric vehicles (EVs) due to their high gravimetric and volumetric energy densities. However, their high-voltage instability (e.g., > 4.3 V vsLi ) limited their usable capacities corresponding to about 60 – 70 % of theoretical capacities. The major problems of high-voltage operation stem from instability of Ni 3+/4+ at cathode-electrolyte interphase (CEI) in contact with electrolytes. Here we propose garnet-type Li 6.7 La 3 Zr 1.7 Ta 0.3 O 12 (LLZT) solid-electrolyte-blended LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC) as high-voltage stable cathodes. The LLZT not only passivates the CEI but scavenges protons and moisture in electrolytes. From well-balanced ionic and electronic transport properties, 5 wt% LLZT blended NMC cathodes delivered enhanced electrochemical performances in full-cells. Unlike other complicated coating processes, our proposed solid-electrolyte blending approach can be readily implementable in commercial Li-ion batteries due to its manufacturing friendliness, energy saving, and cost effectiveness.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2020

High Voltage Surge Protection by a Varistor-Filled Air Gap

The electric discharge across a varistor granule filled air gap under a fast-rising voltage pulse was investigated for surge protection applications. The effects of temperature and pressure on the arc and the electrical conduction were analyzed by the characteristic changes in voltage waveforms triggered by a fast-rising high voltage pulse. In addition to the gap size, experimental results show that competing mechanisms among arc conduction, conduction through the varistor granule network, thermionic emission from Joule heating at granule-to-granule contact points, and the magnitude of the switching voltage dictate the maximum surge protection voltage for the filled air gap. Experimental evidence indicated that accumulated degradation was created at small contact points between varistor granules by repetitive assaults from longer duration, high voltage pulses. The uniqueness of using varistor over other dielectric granules in an air gap for surge protection is identified and discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Oxygen redox activities governing high-voltage charging reversibility of Ni-rich layered cathodes

A schematic illustration indicative of the improved structural reversibility through stabilizing oxidized oxygen by Al doping. The chemical reactions and phase transitions at high voltages are generally considered to determine the electrochemical properties of high-voltage layered cathodes such as Ni-rich rhombohedral oxides. Even if significantly higher SOCs (states-of-charge) are utilized above the capability of transition metal redox (primarily Ni and Co), the effect of oxygen redox on Ni-rich rhombohedral oxides still looks mysterious thereby necessitating research that can clarify the relationship between redox reactions and phase transitions. Here, we performed a comprehensive and comparative study of the cationic and anionic redox reactions, as well as the structural evolution of a series of commercial Ni-rich layered oxides with and without Al doping. We combined the results from X-ray spectroscopy, operando electrochemical mass spectrometry, and neutron diffraction with electrochemical properties and thereby revealed the different oxygen redox activities associated with structural and electrochemical degradations. We reveal that Al doping suppresses the irreversible oxygen release but enhances the lattice oxygen oxidization. With this modulated oxygen redox activity, the Ni-rich layered oxides’ notorious H2–H3 structural phase transition becomes highly reversible. Our findings disentangle the different oxygen redox activities during high-voltage cycling and clarify the role of dopants in the Ni-rich layered oxides in terms of structural and electrochemical stability, shedding light on the future direction of optimizing layered cathode materials for safer high energy-density secondary batteries.

Lee, Gi-Hyeok↗
DOE OSTI2022

Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Oxygen redox at high-voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade, and capacity drop upon cycling; single-crystalline cathodes have recently shown some improvements but these challenges still remain. We reveal the fundamental origin of oxygen redox instability to be originated from the domain boundaries that are present in single-crystalline cathode particles. By synthesizing single-crystalline cathodes free of domain boundaries, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. Further, this leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, and safe batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Impact of Electrolyte Additives on the Lifetime of High Voltage NMC Lithium-Ion Pouch Cells

This work involves improving the lifetime of lithium-ion cells during high voltage cycling using electrolyte additives. Three generations of electrolyte additives were investigated and screened in NMC442/graphite pouch cells using a 24 h voltage-hold protocol at 40 degrees C to accelerate oxidative reactions occurring at 4.4 V. Once promising additives and combinations were identified, they were then tested in cobalt-free NMC640/graphite cells for long-term cycling to upper cutoff voltages of 4.3, 4.4, and 4.5 V at temperatures of 20, 40, and 55 degrees C. Degradation mechanisms were probed using dV/dQ analysis, micro-X-ray fluorescence spectroscopy, and electrochemical impedance spectroscopy. The primary failure mode of cells held at high voltages is due to increase in cell impedance, which is correlated to the dissolution of transition metals, specifically manganese, originating from the positive electrode. We believe this dissolution is presumably due to the formation of a high impedance rock salt surface layer on the NMC positive electrode particles. Such deleterious outcomes can be limited by selecting an appropriate electrolyte additive package. It is hoped that this paper can provide a starting point for developing NMC Li-ion cells that can operate to voltages as high as 4.4 V and still display long lifetimes.

Azam, Saad↗
DOE OSTI2026

High-voltage and electrode system for a cryogenic experiment to search for the neutron electric dipole moment

The cryogenic approach to the search for the neutron electric dipole moment—performing the experiment in superfluid liquid helium—holds promise for a substantial increase in sensitivity, potentially enabling a sensitivity level of 10 −28 𝑒cm. A crucial component in realizing such an experiment is the high-voltage and electrode system capable of providing an electric field of 75 kV/cm. This, in turn, requires an electric potential of 635 kV to be applied to the high-voltage electrode, while simultaneously satisfying other experimental constraints, such as those on heat load and magnetic noise requirements. In this work, we describe the outcome of a comprehensive development program addressing these challenges. It outlines the system requirements, discusses new insights into relevant physical phenomena, and details selected technical solutions with their corresponding experimental demonstrations and expected performance. The results collectively demonstrate the successful development of the necessary technology for the high-voltage and electrode system for this approach.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

An Investigation into High Voltage Spiral Generators Utilizing Thyristor Input Switches

High voltage nanosecond pulses are widely used in scientific research, but their wider adoption in industry requires compact, cost effective and easy to use generators to be developed. This paper presents modelling and experimental investigations into one method of producing such pulses – a spiral generator with a solid-state, thyristor-based input switch. It includes how the pulses are formed within the spiral, why a high speed input switch is required, how the geometry of the spiral dictates its output characteristics, and the effects of different loads. Using thyristors, often connected in series to increase the operating voltage of the spiral, enables the spiral generators to have low jitter, high repetition rate, and long lifetime. Modelling of the circuit used a combination of telegraph equations to account for the wave propagation along the spiral and a lumped circuit exchanging charge between the spiral, the input switch, and the load. The model is verified by detailed experimental results with the relative error being < 10% in most cases. Here, the output voltage pulse was often observed to have an initial peak of much lower magnitude than the subsequent peak(s) – which can only be fully explained by considering wave propagation effects. Lower input switch inductance, shorter switching time, larger mean diameter of the spiral, and increasing the width of the copper tape that makes up the spiral can all increase the voltage multiplication efficiency. Though increasing the number of turns that make up the spiral can increase the output voltage, it can also lower the multiplication efficiency. By understanding the effects of different geometries the spiral can be optimized to drive different loads - three applications of such spiral generators are then presented: pulses with 10 kV amplitude and 10 kHz repetition rate for driving DBD plasma, pulses with amplitude of 10 kV and 10 kV/ns rising rate for triggering of advanced solid state switches, and pulses with -50 kV amplitude and 50 ns rising time for triggering high current gas switches through field distortion.1 Index Terms—spiral generator, nanosecond pulses, telegraph equations, series-connected thyristor module, pulse forming process

42 ENGINEERING↗
DOE OSTI2023

High-voltage monocrystalline Si photovoltaic minimodules based on poly -Si/SiO x passivating contacts for high-power laser power conversion

By using photovoltaic cells under high-intensity laser illumination, much higher photoconversion efficiencies are obtained than under the solar spectrum. Here we demonstrate a monocrystalline Si based minimodule to convert laser light into electricity using edge-illuminated Si "minicells" based on polysilicon on silicon oxide passivating contacts. Ten fully metallized devices were stacked in series and illuminated from the edge, creating a high-voltage, low-current minimodule that mitigates resistive and Auger-Meitner losses. The minimodule shows a high open-circuit voltage of >5 V when tested under 1-Sun illumination and >7 V at higher illumination intensities when tested with a flash simulator. The fill factor in these minimodules is limited by shunting at low illuminations but reaches a maximum of ~78% for higher illumination intensities >40 Suns (current density >1200 mA/cm 2 ), indicating that the minimodules are not limited by series resistance up to 40 Suns. Under 1000 nm monochromatic light, we measure efficiencies >40% at > 40 Suns equivalent illumination, showing the potential of passivated contact Si cells for laser power conversion.

14 SOLAR ENERGY↗
DOE OSTI2021

Long-Term Cycling of a Mn-Rich High-Voltage Spinel Cathode by Stabilizing the Surface with a Small Dose of Iron

The high-voltage, cobalt-free spinel cathode LiNi 0.5 Mn 1.5 O 4 (LNMO) is receiving extensive attention for lithium-ion batteries due to its low cost, high operating voltage and energy density, superior power density, and good thermal stability. However, its high operating voltage hampers its stability with commercial electrolytes and makes its practical viability challenging. We present here a Mn-rich LNMO cathode to encourage the disordering of Mn and Ni in the lattice and the incorporation of a small dose of Fe into Mn-rich LNMO (Fe-LNMO) to improve the cycling stability. The introduction of Fe further increases the cation disorder between Mn and Ni, thus enabling a better rate capability. Electron energy loss spectroscopy analysis indicates that Fe is concentrated on the surface, and X-ray photoelectron spectroscopy analysis shows that Fe-LNMO alleviates the aggressive reaction between the cathode surface and the electrolyte, thus stabilizing the interface and cycle life. Furthermore, a full cell assembled with a graphite anode with an areal capacity of 3 mA h cm –2 displays a capacity retention of 90% over 300 cycles. Furthermore, the present work demonstrates an effective way to promote cation disordering and lower the surface reactivity of LNMO with the electrolyte, thereby enhancing the conductivity, stabilizing the cathode–electrolyte interphase, and making LNMO promising for practical applications.

25 ENERGY STORAGE↗