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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Kinetically Dormant Ni‐Rich Layered Cathode During High‐Voltage Operation

Abstract The degradation of Ni‐rich cathodes during long‐term operation at high voltage has garnered significant attention from both academia and industry. Despite many post‐mortem qualitative structural analyses, precise quantification of their individual and coupling contributions to the overall capacity degradation remains challenging. Here, by leveraging multiscale synchrotron X‐ray probes, electron microscopy, and post‐galvanostatic intermittent titration technique, the thermodynamically irreversible and kinetically reversible capacity loss is successfully deconvoluted in a polycrystalline LiNi 0.83 Mn 0.1 Co 0.07 O 2 cathode during long‐term charge/discharge cycling in full cell configuration. Contradicting the dramatic capacity loss, the layered structure remains highly alive even after 1000 cycles at 4.6 V while undergoing a three‐order of magnitude reduction in the mass transfer kinetics, leading to almost fully recoverable capacity under kinetic‐free conditions. Such kinetic dormant behavior after cycling is not simply ascribed to poor chemical diffusion by reconstructed cathode surface but highly synchronizes with the lattice strain evolution stemming from the structural heterogeneity between deeply delithiated layered and degraded rock‐salt phases at high voltage. These findings deepen the degradation mechanism of high‐voltage cathodes to achieve long‐cycling and fast‐charging performance.

36 MATERIALS SCIENCE↗
DOE OSTI2024

A Green, Fire–Retarding Ether Solvent for Sustainable High–Voltage Li–Ion Batteries at Standard Salt Concentration

Lithium-ion batteries (LIBs) are increasingly encouraged to enhance their environmental friendliness and safety while maintaining optimal energy density and cost-effectiveness. Although various electrolytes using greener and safer glyme solvents have been reported, the low charge voltage (usually lower than 4.0 V vs Li/Li + ) restricts the energy density of LIBs. Herein, tetraglyme, a less-toxic, non-volatile, and non-flammable ether solvent, is exploited to build safer and greener LIBs. It is demonstrated that ether electrolytes, at a standard salt concentration (1 m), can be reversibly cycled to 4.5 V vs Li/Li + . Anchored with Boron-rich cathode-electrolyte interphase (CEI) and mitigated current collector corrosion, the LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode delivers competitive cyclability versus commercial carbonate electrolytes when charged to 4.5 V. Synchrotron spectroscopic and imaging analyses show that the tetraglyme electrolyte can sufficiently suppress the overcharge behavior associated with the high-voltage electrolyte decomposition, which is advantageous over previously reported glyme electrolytes. The new electrolyte also enables minimal transition metal dissolution and deposition. NMC811||hard carbon full cell delivers excellent cycling stability at C/3 with a high average Coulombic efficiency of 99.77%. In conclusion, this work reports an oxidation-resilient tetraglyme electrolyte with record-high 4.5 V stability and enlightens further applications of glyme solvents for sustainable LIBs by designing Boron-rich interphases.

36 MATERIALS SCIENCE↗
DOE OSTI2025

A Reductively Stable Electrolyte Realizes Deep Cycling Behavior in Anode‐free Sodium Batteries

For anode‐free sodium batteries to achieve practical consideration, highly reversible chemistries require exceptional ≥99.95% coulombic efficiencies that maintain over prolonged cycling periods. To do so, consumption of this severely limited sodium inventory must be restricted while metal nucleation processes that comprise the in situ formed metal anode are improved. Herein, we describe a fluorine‐free carborane electrolyte that satisfies these criteria by emphasizing reductive stability and weakly coordinating anion behavior as design principles. We find this approach promotes the development of a thin, robust SEI chemistry rich in both organic speciation and boron. The electrolyte described herein exhibits ideal metal nucleation behavior on one‐micron thin carbonaceous current collector surfaces and achieves a metal deposition/stripping efficiency near parity for 400 cycles. This novel anode chemistry is introduced to anode‐free full cell configurations where 87% of the initial discharge capacity is retained after 1000 cycles at 2.0 C. In conclusion, post‐test characterization of deep‐cycled anode‐free cells reveals suppressed capacity fade in these systems is attributed to the chemical stability of the carborane anion.

anode-free↗
DOE OSTI2024

Multiple Functional Bonds Integrated Interphases for Long Cycle Sodium-Ion Batteries

Sodium-ion batteries (SIBs) have garnered significant interest as one of the most promising energy suppliers for power grid energy storage. However, the poor electrode/electrolyte interfacial stability leads to continual electrolyte decomposition and transition metal dissolution, resulting in rapid performance degradation of SIBs. In this work, we propose a strategy integrating multiple functional bonds to regulate electrode/electrolyte interphase by triple-coupling of succinonitrile (SN), sodium hexafluorophosphate (NaPF 6 ) and fluorinated ethylene carbonate (FEC). Theoretical calculation and experiment results show that the solvation structure of Na + and ClO 4 – is effectively reconfigured by the solvated FEC, SN and PF 6 – in PC-based carbonate electrolyte. The newly developed electrolyte demonstrates increased Na + -FEC coordination, weakened interaction of Na + -PC and participation of SN and PF 6 – anions in solvation, resulting in the formation of a conformal interfacial layer comprising of sodium oxynitrides (NaN x O y ), sodium fluoride (NaF) and phosphorus oxide compounds (NaP x O y ). Consequently, a 3 Ah pouch full cell of hard carbon//NaNi 1/3 Fe 1/3 Mn 1/3 O 2 exhibits an excellent capacity retention of 90.4 % after 1000 cycles. Detailed postmortem analysis of interface chemistry is further illustrated by multiple characterization methods. Finally, this study provides a new avenue for developing electrolyte formulations with multiple functional bonds integrated interphases to significantly improve the long-term cycling stability of SIBs.

25 ENERGY STORAGE↗
DOE OSTI2024

In Situ Alloying Enabled by Active Liquid Metal Filler for Self‐Healing Composite Polymer Electrolytes

Abstract Solid inorganics, known for kinetically inhibiting polymer crystallization and enhancing ionic conductivity, have attracted significant attention in solid polymer electrolytes. However, current composite polymer electrolytes (CPEs) are still facing challenges in Li metal batteries, falling short of inhibiting severe dendritic growth and resulting in very limited cycling life. This study introduces Ga 62.5 In 21.5 Sn 16 (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self‐healing protection against dendrite problems. Compared to solid inorganics, for example silica, LM droplets could more significantly reduce polymer crystallinity and enhance Li‐ion conductivity due to their liquid nature, especially at temperatures below the polymer melting point. More importantly, LMs are unraveled as dynamic chemical traps, which are capable of blocking and consuming lithium dendrites upon contact via in situ alloying during battery operation and further inhibiting dendritic growth due to the lower deposition energy barrier of the formed Li‐LM alloy. As a proof of concept, by strategically designing an asymmetric CPE with the active LM filling, a solid‐state Li/LiFePO 4 battery achieves promising full‐cell functionality with notable rate performance and stable cycle life. This active filler‐mediated self‐healing approach could bring new insights into the battery design in versatile solid‐state systems.

Wu, Kai↗
DOE OSTI2025

Anionic‐Based Layered Oxide Cathodes with High Electrochemical Performance through Dual‐Site Substitutions for Sodium‐Ion Batteries

Mn-rich layered oxide cathodes with anionic redox promise high energy density for sodium-ion batteries (SIBs) due to ultra-high capacity derived from both Mn and O redox couples. Nevertheless, instability of the reactions that lead to poor electrochemical stability hinders the cathodes from practical applications. Here, the Al and Zn dual-site substitution strategy is proposed to enhance electrochemical performance. Here, the designed cathode, Na 0.73 Zn 0.03 Li 0.25 Mn 0.76 Al 0.01 O 2 (AlZn), delivers a high discharge capacity of 242 mAh g −1 with an impressive rate capability (162 mAh g −1 at 1000 mA g −1 ) and excellent capacity retention (89.69% over 150 cycles). In addition, full-cell SIB based on AlZn coupled with hard carbon exhibits a high energy density of 317 Wh kg −1 (based on both cathode and anode mass) and a reasonable capacity retention of 80.8% after 250 cycles. Revealed by advanced investigations, the synergy of robust Al–O in TM layers and O–Zn–O pillars in Na layers helps alleviate severe inactive spinel/rock-salt phase transformation and intragranular cracks in the AlZn cathode. This consequently leads to greatly enhanced electrochemical performance over the pristine cathode. This work provides insight into improving electrochemical properties of anionic-redox-based layered oxides by Al/Zn co-substitutions toward high-energy SIBs.

25 ENERGY STORAGE↗
DOE OSTI2025

Micron Size NaCrO 2 Particles Enable High‐loading Dry‐processed Electrode for Sodium Ion Batteries

Dry-process fabrication using fibrillatable binder is emerging as a promising method to produce high-loading electrodes for energy storage applications, favored by its cost-efficiency and eco-friendliness. While previous studies have demonstrated the advantages of dry process over the traditional slurry method, there remains a gap in understanding how the particle size of active materials influences the mechanical and electrochemical performance of dry electrodes. In this study, four different particle size NaCrO 2 materials (Average size, S-NCO: 0.6 µm, M1-NCO 1.5 µm, M2-NCO: 4.4 µm, and L-NCO: 9.9 µm) are synthesized to investigate the effect of particle size on dry-processed high-loading electrodes. The findings reveal that the larger micron-sized (>4.4 µm) NCO dry films exhibit significantly improved tensile strength and electrochemical performance, primarily ascribed to the low film porosity, abundant inter-particle connection by the binder, comprehensive carbon coverage, and efficient percolation of the conductive pathway. Notably, a full cell incorporated with a high loading (5.2 mAh cm −2 ) and high active material ratio (96.5 wt.%) L-NCO film electrode demonstrates promising cycling stability and rate capability. Furthermore, these results provide valuable insights regarding the design and fabrication of dry-processed electrodes for future energy storage applications.

25 ENERGY STORAGE↗
DOE OSTI2026

Interfacial and Kinetic Origins of Voltage Loss in Neutral Zinc‐Air Batteries

Rechargeable zinc-air batteries are promising candidates for grid-scale energy storage; however, their practical deployment is limited by oxygen electrocatalysis inefficiencies and interfacial instabilities, particularly outside conventional alkaline electrolytes. Here, in this work, zinc-air batteries operating under neutral electrolyte conditions using ZnCl 2 soaked KC-PAA-PAM gel polymer electrolytes and electrochemically synthesized Ni/Fe layered double hydroxide electrocatalysts is investigated. Ni/Fe-LDH is intentionally employed as an OER-biased benchmark catalyst to diagnose electrolyte and interface driven limitations rather than as a bifunctional ORR/OER solution. Full cells exhibit highly stable cycling over hundreds of hours, yet operate at substantially suppressed charge and discharge voltages relative to the thermodynamic value. Electrochemical impedance analysis shows that ohmic losses contribute only minimally to this voltage suppression. Post-mortem X-ray photoelectron spectroscopy reveals metallic zinc accumulation on the air cathode and chloride-containing species on the anode, indicating parasitic interfacial processes. Synchrotron-based soft X-ray absorption spectroscopy confirms stable Ni 2+ and Fe 3+ oxidation states during cycling, consistent with OER-biased catalytic behavior, while neutral-electrolyte oxygen evolution measurements demonstrate strong electrolyte-induced suppression of oxygen kinetics. Together, these results show that electrolyte chemistry and cathode-side parasitic processes, rather than catalyst identity alone, dominate voltage losses in neutral zinc-air batteries, providing mechanistic insight into the fundamental challenges associated with neutral electrolyte operation.

Long duration energy storage↗
DOE OSTI2024

Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Roll-to-roll powder-to-film dry processing (DP) and single-crystal (SC) active materials (AMs) with many advantages are two hot topics of lithium-ion batteries (LIBs). However, DP of SC AMs for LIBs is rarely reported. Consequently, the impact of SC AMs on dry-processed LIBs is not well understood. Herein, for the first time, via a set of experimental and theoretical studies of the conventional polycrystalline-AM- and SC-AM-based DPed electrodes (DPEs), this work not only reports a high-performance dry SC-AM cathode for LIB manufacturing, but also establishes some fundamental understanding of SC-based dry-processed electrodes, including their morphology, structure, mechanical strength, electronic conductivity and LIB electrochemical behavior. Further, the results suggest that DP of SC AMs is promising, which can dramatically improve the electrochemical kinetics at electrode level and particle level. Specifically, for the rate capability and long-term cyclability in full cells, SC DPEs exhibit a discharge specific capacity of 152.1 mAh g -1 at 1C and a capacity retention rate of 79.9 % at C/3 over 500 cycles, which are superior to those of PC DPEs (135.6 mAh g -1 and 68.3 %) at the same conditions and are further confirmed by the simulation data from the theoretical modelling study. Therefore, this comprehensive work marks a significant milestone for DP strategy and SC AMs, enlightening future research and development of LIB manufacturing.

25 ENERGY STORAGE↗
DOE OSTI2025

Integration of hydrophobic gas diffusion layers for zero-gap electrolyzers to enable highly energy-efficient CO 2 electrolysis to C 2 products

Electrochemical CO 2 reduction (eCO2R) is an attractive route for mitigating global CO 2 emissions while producing value-added chemicals. Ethylene is one product of eCO2R and is an essential industrial precursor with a global market of $230 billion. The large-scale implementation of C 2 H 4 -selective CO 2 electrolyzers remains challenging because of low energy efficiencies. In this work, we develop the design principles necessary for incorporating an expanded polytetrafluoroethylene (ePTFE) electrode into a zero-gap electrolyzer while simultaneously developing an integrated electrical front contact that reduces the ohmic resistances inherent to electrically insulating gas diffusion layers. By co-designing the catalyst layer, gas diffusion medium, and operating conditions for a zero-gap ePTFE gas diffusion electrode (GDE), we achieved a full-cell voltage of 2.5 V at 200 mA cm −2 at 25 cm 2 geometric area cell with Faradaic efficiencies of 48% for ethylene and 40% for ethanol. This work highlights strategies for developing a scalable, stable, and highly energy-efficient eCO2R for C 2 products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Impact of anion-exchange membrane degradation on long-term CO 2 electrolysis to ethylene

Electrochemical CO 2 reduction (eCO2R) to ethylene offers a unique opportunity to diversify domestic supply chains for chemical manufacturing. Large-scale deployment of eCO2R to ethylene reactors is currently limited by low energy efficiencies and poor durability. Herein, we demonstrate >100 h of continuous electrolysis at an industrially relevant current density of 200 mA cm −2 in a 25 cm 2 geometric area zero-gap reactor with a full-cell voltage <3.1 V and ethylene Faradaic efficiency >30%. Incorporating expanded polytetrafluoroethylene (PTFE)-supported electrodes into zero-gap reactors allows for durable electrode catalysts that are resistant to flooding, and this enables wider ranges of operating parameters not typically accessible in CO 2 electrolysis. Finally, we identify membrane degradation, evidenced by a loss of membrane ion-exchange capacity, as the leading cause of performance loss over 144 h of electrolysis.

Energy - Conversion↗
DOE OSTI2025

Enabling fast-charging of lithium-ion batteries through printed electrodes

It has been well recognized that introducing secondary porous networks (SPNs) into the electrodes can effectively improve the electrochemical performance of lithium-ion batteries (LIBs), especially under fast-charging operations. However, the process complexity and high cost limit the commercial success of advanced electrodes with SPNs. To address this issue, we developed a facile screen-printing process to produce structured graphite electrodes with SPNs. The experimental results demonstrated that, by tuning the diameter and center-to-center (C2C) distance of emulsion dots on the stencil screen, the pore diameters and C2C pore distances of SPNs in screenprinted electrodes can be precisely controlled in the range of 100 mu m to 1 mm and 100 mu m to 3 mm respectively. In addition, the SPNs with hexagonal and square-shape pore alignments have also been imprinted onto the electrode coatings through adjusting the patterns of screen stencils. Used as anodes, the printed graphite electrodes demonstrated significantly reduced overpotential and voltage fluctuation under fast-charging operations from 2C to 6C. Coupled with LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) cathodes, the full cells with printed graphite anodes exhibited an unprecedently stable performance with almost no capacity decay up to 170 cycles when charged to 80 % SOC at 2C. Observations from electron microscopy showed plated lithium undetectable at the surface of printed graphite electrodes after numerous cycles. The electrochemical analysis on the voltage evolution during the cell rest period indicated the significantly delayed onset of lithium plating in the presence of printed graphite electrodes. In conclusion, all these results suggest that the significantly improved cell performance is associated with the shortened Li-ion diffusion distance, reduced polarization and suppressed Li plating in the printed electrodes with patterned SPNs.

25 ENERGY STORAGE↗
DOE OSTI2026

Zinc treatment to enhance nickel electrode performance for liquid alkaline water electrolyzers

Raney Ni treatment is introduced to the surface of Ni mesh anode electrodes, enhancing liquid alkaline water electrolyzer performance. The surface of the Ni mesh is alloyed with Zn, deposited by either an aqueous infiltration of Zn salt or direct reaction with Zn foil. The extent of alloying is controlled by a heat treatment step. For both processes, fine porosity and enhanced surface area are obtained after leaching the Zn out of the surface alloy layer. The observed electrode surface structure and performance is quite sensitive to the thermal treatment temperature. The enhanced surface area improves full cell performance by 90 mV for infiltrated Zn treated at 600 °C and by 185 mV for Zn foil reacted at 425 °C (at 2 A cm −2 and 80 °C). In conclusion, the Zn treatment methods produce stable operating performance, exhibiting no decay after 150 h for the infiltrated Zn treated at 600 °C, and a decay rate of 4.6 μV h −1 over 100 h for the Zn foil reacted at 425 °C (at 1 A cm −2 and 80 °C).

LAWE↗
DOE OSTI2024

A reversible four-electron Sn metal aqueous battery

Sn is a promising metal anode for aqueous batteries, with up to four-electron redox available per atom (903 mAh g −1 Sn ). However, practically harnessing the four-electron Sn(OH) 6 2− /Sn reversibility remains challenging due to limited mechanistic understanding. Here, in this study, we reveal a kinetically asymmetric redox pathway involving a successive four-electron plating and a stepwise 2 + 2 electron stripping through a Sn(OH) 3 − intermediate. The crossover of Sn(OH) 3 − induces a reversible self-discharge that reduces Coulombic efficiency but does not impact cyclability, demonstrated by four-electron Sn-Ni full cells that sustain >800 h of stable cycling. By tuning the ion selectivity of the separator to suppress Sn(OH) 3 − crossover while allowing OH − transport, we further demonstrate high Sn utilization (67%) and high energy density (143.1 Wh L −1 cell). The results provide key understandings of the tradeoffs in engineering reversible multi-electron metal anodes and define a new benchmark for practical energy density that exceeds any Sn-based aqueous batteries to date.

SN anode↗
DOE OSTI2025

In-situ formation of stable interface towards Li-in anode for halide solid-state electrolyte

Halide-based solid-state electrolytes (SSEs) are promising candidates for next-generation all-solid-state lithium batteries (ASSLBs) due to their high ionic conductivity and chemical stability. However, their poor interfacial compatibility with lithium metal anode and Li-In alloy significantly hinder practical application due to the requirement for a protective interlayer. In this study, a novel approach to overcome this limitation is presented by introducing iron (Fe) doping into Li 3 InCl 6 (LIC), which enables direct and stable contact with lithium-indium (Li-In) metal without a protective interlayer. Thermodynamic and computational analyses identified Fe 3+ as a suitable dopant based on its similar reduction potential to In 3+ and structural compatibility within the halide lattice. The synthesized 10 at. % Fe-doped LIC exhibits high phase purity, retained ionic conductivity, and notably improved interfacial stability. Full-cell tests using Fe-LIC achieve over 300 cycles with 80 % capacity retention. At the same time, symmetric Li-In/ Fe-LIC/ Li-In cells sustain over 500 h of operation, representing the first reported long-term cycling of LIC-based ASSLB without a protective interlayer. In conclusion, this work establishes Fe doping as an effective strategy to stabilize halide SSEs of In system against Li-In alloy, thereby simplifying cell architecture and advancing the development of safer, high-performance halide-based solid-state electrolytes.

Halide-based solid-state electrolytes↗
DOE OSTI2024

Mitigating Calendar Aging in Si-NMC Batteries with Advanced Dual-Salt Glyme Electrolytes

In addressing the critical challenge of calendar aging in silicon (Si)-based lithium-ion batteries, this study introduces a groundbreaking strategy utilizing glyme-type dual-salt electrolytes (lithium bis(trifluoromethanesulfonyl)imide [LiTFSI] and lithium difluoro(oxalato)borate [LiDFOB]). These electrolytes are demonstrated to significantly mitigate parasitic reactions and capacity loss in Si-NMC (lithium nickel manganese cobalt oxide) full cells, especially when compared with traditional carbonate-based electrolytes. Further, our exhaustive mechanistic analysis reveals that such electrolytes not only preserve the integrity of the Si anode but also improve the cathode/electrolyte interphases (CEI) through the formation of a conformal coating on the high-voltage cathode surface. This dual-salt approach, enhanced by the addition of a phosphate additive, effectively decelerates calendar aging, marking a substantial advance in the quest for durable and reliable Si-based energy storage technologies. The findings underscore the vital role of electrolyte composition in extending the calendar life of Si batteries, offering an alternative avenue toward maximizing the performance and longevity of next-generation Li-Si batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2024

The Impact of Lithium Anode Interface on Capacity Fade in Polymer Electrolyte-Based Solid-State Batteries

This study investigates the Li stripping-plating morphology and failure mechanisms in full cells consisting of a solid polymer electrolyte (SPE) with two commercial Li anodes: Li chip and Li foil. The primary identified failure mechanism of the SPE cell is capacity fade, regardless of the Li manufacturer. While the cathode’s role in capacity fade is evident, the Li anode significantly influences cycling performance, with Li foil cells cycling 50% longer than Li chip cells, a statistical difference. Further, post-mortem scanning electron microscopy and X-ray photoelectron spectroscopy results attribute the Li chip’s faster capacity fade to a loss of contact and continuous growth of the solid electrolyte interphase (SEI). Conversely, Li foil maintains consistent contact with the solid polymer, displaying a thin and stable SEI. Additionally, failure mechanisms between a gel electrolyte in previous work and the dry SPE are compared.

25 ENERGY STORAGE↗
DOE OSTI2025

Quaternary Cu 2 TSiS 4 (T = Fe, Mn) Anodes for Li-Ion Batteries

Developing high-capacity and fast-charging anode materials is critical for achieving high-performance Li-ion batteries (LIBs). Herein, polycrystalline quaternary transition metal silicon sulfides, Cu 2 TSiS 4 (T = Fe, Mn), were synthesized using a solid-state method and investigated as anode materials in LIBs. Cu 2 FeSiS 4 retains a reversible capacity of 670 mAh g –1 at 200 mA g –1 for 400 cycles, while Cu 2 MnSiS 4 suffers from a fast capacity loss in the initial 50 cycles. More importantly, Cu 2 FeSiS 4 can maintain a reversible capacity of 379 mAh g –1 after 700 cycles at a high current density of 2 A g –1 , demonstrating high cyclic stability and fast-charging capacity. To further understand the structure degradation and phase transformation, we investigated the postcycling electrodes using multiple techniques, including the scanning electron microscope with energy-dispersive X-ray spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy techniques. The results indicated that Cu 2 FeSiS 4 undergoes reversible phase transitions with Li 2 S as a major product component. To further assess the performance for practical applications, Cu 2 FeSiS 4 was coupled with LiFePO 4 to make LiFePO 4 ||Cu 2 FeSiS 4 full cells, which delivered superior electrochemical performance. These results demonstrate great promise for using quaternary transition metal silicon sulfides as anodes to achieve low-cost and sustainable LIBs.

25 ENERGY STORAGE↗