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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Anomalously high elastic modulus of a poly(ethylene oxide)-based composite electrolyte

The practical use of lithium metal anodes in solid-state batteries requires a polymer membrane with high lithium-ion conductivity, thermal/electrochemical stability, and mechanical strength. The primary challenge is to effectively decouple the ionic conductivity and mechanical strength of the polymer electrolytes. We report a remarkably facile single step synthetic strategy based on in-situ crosslinking of poly(ethylene oxide) (xPEO) in the presence of a woven glass fiber (GF). Such a simple method yields composite polymer electrolytes (CPE) of anomalously high elastic modulus up to 2.5 GPa over a broad temperature range (20 °C – 245 °C) that has never been previously documented. An unsupervised machine learning algorithm, K-mean clustering analysis, was implemented on the hyperspectral Raman mapping at the xPEO/GF interface. Using such a unique means, we show for the first time that the promoted mechanical strength originates from xPEO and GF interactions through dynamic hydrogen and ionic bonding. High ionic conductivity is achieved by the addition plasticizer (e.g. tetraglyme), where trifluoromethanesulfonate anions are tethered to the xPEO matrix and Li + cations are favorably transported through coordination with the plasticizer. Further, stringent galvanostatic cycling tests indicates the CPE can be stably cycled for >3000 h in a Li-metal symmetric cell at a moderate temperature (nearly 1500 Coulombs/cm 2 Li equivalents), outperforming most of the PEO-based electrolytes. The GF reinforced CPE reported here has multifunctional uses, such as solid electrolytes for all solid-state batteries and membranes for redox-flow batteries. Although the focus of this study is on lithium-based batteries, the results are equally promising for other alkali metal based batteries such as sodium and potassium.

25 ENERGY STORAGE↗
DOE OSTI2021

Process for fabrication of enhanced β″-alumina solid electrolytes for energy storage devices and energy applications

A dense β″-alumina/zirconia composite solid electrolyte and process for fabrication are disclosed. The process allows fabrication at temperatures at or below 1600° C. The solid electrolytes include a dense composite matrix of β″-alumina and zirconia, and one or more transition metal oxides that aid the conversion and densification of precursor salts during sintering. The composite solid electrolytes find application in sodium energy storage devices and power-grid systems and devices for energy applications.

Lu, Xiaochuan↗
DOE OSTI2023

Delineating the Impact of Transition‐Metal Crossover on Solid‐Electrolyte Interphase Formation with Ion Mass Spectrometry

Abstract Lithium‐metal batteries (LMB) employing cobalt‐free layered‐oxide cathodes are a sustainable path forward to achieving high energy densities, but these cathodes exhibit substantial transition‐metal dissolution during high‐voltage cycling. While transition‐metal crossover is recognized to disrupt solid‐electrolyte interphase (SEI) formation on graphite anodes, experimental evidence is necessary to demonstrate this for lithium‐metal anodes. In this work, advanced high‐resolution 3D chemical analysis is conducted with time‐of‐flight secondary‐ion mass spectrometry (TOF‐SIMS) to establish spatial correlations between the transition metals and electrolyte decomposition products found on cycled lithium‐metal anodes. Insights into the localization of various chemistries linked to crucial processes that define LMB performance, such as lithium deposition, SEI growth, and transition‐metal deposition are deduced from a precise elemental and spatial analysis of the SEI. Heterogenous transition‐metal deposition is found to perpetuate both heterogeneous SEI growth and lithium deposition on lithium‐metal anodes. These correlations are confirmed across various lithium‐metal anodes that are cycled with different cobalt‐free cathodes and electrolytes. An advanced electrolyte that is stable to higher voltages is shown to minimize transition‐metal crossover and its effects on lithium‐metal anodes. Overall, these results highlight the importance of maintaining uniform SEI coverage on lithium‐metal anodes, which is disrupted by transition‐metal crossover during operation at high voltages.

Chemistry↗
DOE OSTI2021

Li 2 S 6 ‐Integrated PEO‐Based Polymer Electrolytes for All‐Solid‐State Lithium‐Metal Batteries

Abstract The integration of Li 2 S 6 within a poly(ethylene oxide) (PEO)‐based polymer electrolyte is demonstrated to improve the polymer electrolyte's ionic conductivity because the strong interplay between O 2− (PEO) and Li + from Li 2 S 6 reduces the crystalline volume within the PEO. The Li/electrolyte interface is stabilized by the in situ formation of an ultra‐thin Li 2 S/Li 2 S 2 layer via the reaction between Li 2 S 6 and lithium metal, which increases the ionic transport at the interface and suppresses lithium dendrite growth. A symmetric Li/Li cell with the Li 2 S 6 ‐integrated composite electrolyte has excellent cyclability and a high critical current density of 0.9 mA cm −2 at 40 °C. Impressive electrochemical performance is demonstrated with all‐solid‐state Li/LiFePO 4 and high‐voltage Li/LiNi 0.8 Mn 0.1 Co 0.1 O 2 cells at 40 °C.

Fang, Ruyi↗
DOE OSTI2025

Modulating physicochemical interfaces enables li-rich oxides based ceramic solid-state li batteries under ambient conditions

Li-rich layered oxides exhibit promising potential applications in high-energy-density solid-state lithium metal batteries. Nevertheless, the strong oxidative oxygen species generate at high voltage, which poses great challenges to positive electrode-side interface stability. Herein, a robust in-situ polymerization gel polymer electrolyte with bifunctional additives is designed for interface modification. These additives, include lithium difluoro(oxalate) borate and LiPO 2 F 2 , regulate the Li + chemical environment in gel polymer electrolyte to enhance crosslink density without residual oligomer, which reduce gas generation and suppress contact loss, thus avoiding interfacial impedance divergence. Concurrently, the designed gel polymer electrolyte enables a wide electrochemical stability window (up to 4.7 V) and a high Li + transference number (0.82). Additionally, the additives induced F- and B-rich inorganic cathode-electrolyte interphase inhibits side reactions and oxygen/transition metal loss effectively, stabilizing the chemical interface. The as-constructed Li-rich layered oxides-based ceramic solid-state lithium metal batteries with gel polymer electrolyte interface modification exert a high discharge capacity of 276.5 mAh g -1 at 30 °C without external pressure, delivering a retention of 81.7% after 100 cycles at 25 mA g -1 during 2.0-4.7 V. This work provides a guideline for developing high-voltage solid-state lithium metal batteries via interfacial design.

Hu, Xinchao [Xiamen University (China)]↗
DOE OSTI2020

Enhanced Surface Interactions Enable Fast Li + Conduction in Oxide/Polymer Composite Electrolyte

Abstract Li + ‐conducting oxides are considered better ceramic fillers than Li + ‐insulating oxides for improving Li + conductivity in composite polymer electrolytes owing to their ability to conduct Li + through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li + ‐insulating oxides (fluorite Gd 0.1 Ce 0.9 O 1.95 and perovskite La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 2.55 ) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)‐based polymer composite electrolytes, each with a Li + conductivity above 10 −4 S cm −1 at 30 °C. Li solid‐state NMR results show an increase in Li + ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2‐site occupancy originates from the strong interaction between the O 2− of Li‐salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li + transport. All‐solid‐state Li‐metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C.

Wu, Nan↗
DOE OSTI2023

Achieving stable all-solid-state lithium-metal batteries by tuning the cathode-electrolyte interface and ionic/electronic transport within the cathode

All-solid-state batteries with sulfide electrolytes and high-nickel layered oxide cathodes attract much interest due to their high specific energy. However, their cycling performance is primarily influenced by the interface between the sulfide electrolyte and the high-Ni layered oxide particles, which requires the use of composite cathodes with high ionic and electronic conductivities to achieve a kinetically stable interface inside the cathode. Here, we apply Ti 2 O 3 particles to the high-Ni cathode LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), where Ti 2 O 3 not only acts as an electronic conductor to provide a fast diffusion path for electrons in the composite cathode, but also absorbs the lattice oxygen released from NCM811 cathode during cycling, stabilizing the Li 6 PS 5 Cl/NCM811 interface and suppressing electrolyte oxidation. The as-modified cathode exhibits an initial specific capacity of 192 mAh g -1 and retains 166 mAh g -1 after 140 cycles at 0.1C rate with a good capacity retention of 86.5%. Furthermore, the composite cathode displays high rate capability even at 1C rate. By contrast, the unmodified Li 6 PS 5 Cl/NCM811 cathode shows poor cycling performance with only 130 mAh g -1 remaining after 130 cycles. This work provides a new direction for the design of cathodes for all-solid-state batteries that can deliver high specific energy with long cycle life.

25 ENERGY STORAGE↗
DOE OSTI2025

Rapid scalable plasma processing of thin-film Li–La–Zr–O solid-state electrolytes

Solid-state electrolytes, such as lithium lanthanum zirconium oxide (LLZO), show promise as technologies for next-generation high-energy-density batteries, but commercial development has been hindered by a lack of scalable processing methods. Current fabrication methods are costly or require long annealing steps to create dense films. We report an atmospheric pressure blown-arc nitrogen plasma jet process to rapidly form sub-micrometer-thick, dense amorphous LLZO (a-LLZO) films from sol-gel precursors. Films are processed in less than 2 min, an order of magnitude faster than what has previously been reported. We demonstrate 500-nm-thick a-LLZO films processed at 350°C with an ionic conductivity of 2 × 10 −6 S/cm at 30°C and 2 × 10 −3 S/cm at 100°C and a conductance of 19 S at 100°C, the highest conductance of any LLZO phase to date. Here, the films exhibit outstanding smooth surface morphology with low defectivity, advancing atmospheric plasma processing as a scalable processing method for solid-state electrolytes.

25 ENERGY STORAGE↗
NASA NTRS2006

Miniature Oxidizer Ionizer for a Fuel Cell

A proposed miniature device for ionizing the oxygen (or other oxidizing gas) in a fuel cell would consist mostly of a membrane ionizer using the same principles as those of the device described in the earlier article, Miniature Bipolar Electrostatic Ion Thruster (NPO-21057). The oxidizing gas would be completely ionized upon passage through the holes in the membrane ionizer. The resulting positively charged atoms or molecules of oxidizing gas could then, under the influence of the fringe fields of the ionizer, move toward the fuel-cell cathode that would be part of a membrane/electrode assembly comprising the cathode, a solid-electrolyte membrane, and an anode. The electro-oxidized state of the oxidizer atoms and molecules would enhance transfer of them through the cathode, thereby reducing the partial pressure of the oxidizer gas between the ionizer and the fuel-cell cathode, thereby, in turn, causing further inflow of oxidizer gas through the holes in the membrane ionizer. Optionally the ionizer could be maintained at a positive electric potential with respect to the cathode, in which case the resulting electric field would accelerate the ions toward the cathode.

Hartley, Frank↗
NASA NTRS1978

Long-lasting solid-polymer electrolytic hygrometer

Device consists of hollow tube node of oxidation-resistant sulfonated fluorocarbon polymer. Tube absorbs moisture from air passing across inner and outer surfaces, causing change in polymer conductance. Change is related to change in water content in gas sample.

Lawson, D. D.↗
DOE OSTI2021

All solid thick oxide cathodes based on low temperature sintering for high energy solid batteries

Solid-state batteries (SSBs) could significantly improve the safety and energy density over conventional liquid cells. One key enabling technology is the use of solid electrolytes. NASICON-type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) is a very attractive solid-state electrolyte for the cathode side due to its high oxidation potential and high ionic conductivity. The usage, however, is limited by its large interfacial resistance against most of the cathode materials as well as the thermodynamic instability during high temperature sintering needed to achieve high mass density. Here we construct thin, percolative, and mixed conductive interphases through in situ low-melting-point liquid sintering. These mixed conductive interphases drastically improve the kinetics, leading to high-loading solid LATP/LiCoO 2 cathodes achieving capacity loading of up to ~6 mA h cm –2 . The technique is also applicable to Ni-rich cathode materials, achieving up to ~10 mAh cm –2 , which can lead to more than 400 W h kg –1 cells in SSBs. Furthermore, our composite cathodes show a ten-times and three-times area capacity improvement over the state-of-the-art cathodes using oxide and sulfide SSEs, respectively.

25 ENERGY STORAGE↗
DOE OSTI2022

Electrolyzers for Hydrogen Production: Solid Oxide, Alkaline, and Proton Exchange Membrane

The effects of climate change have led to a push for cleaner energy sources across multiple sectors. Hydrogen has emerged as a promising energy carrier in this context, as it can be produced using various water electrolysis technologies capable of utilizing clean power (e.g., nuclear and renewable electricity). However, a comprehensive environmental assessment of these technologies requires an understanding of the environmental impacts during their complete life cycle, including the embodied emissions in their material composition and during their manufacturing stages; these emissions are often neglected. This report provides a brief overview of major water electrolysis technologies, viz., proton exchange membrane electrolyzer cell (PEMEC) or polymer electrolyte membrane (PEM), alkaline electrolysis cell (AEC) and solid oxide electrolysis cell (SOEC), along with a detailed bill of materials for these technologies that has been incorporated in the updated G reenhouse gases, R egulated E missions, and E nergy use in T ransportation (GREET ® ) 2022 model. We also provide an inventory for the intermediate materials used to produce these electrolyzers, which has not been covered in prior releases. Using these material and energy flows, the GREET model provides a detailed life cycle inventory (energy use and emissions) from raw material extraction through complete production of electrolyzers for major electrolysis technologies.

08 HYDROGEN↗
DOE OSTI2025

Ion Size Effects on the Thermodynamic, Kinetic, and Mechanical Properties during Ion Exchange in Solid-State Electrolytes

Ion exchange offers a pathway to impose residual compressive stresses to mitigate the electro-chemo-mechanical cracking of solid-state electrolytes such as lithium lanthanum zirconium oxide. This study uses a coupled multiscale framework (integrating density functional theory (DFT), molecular dynamics (MD), and continuum modeling) to examine how exchange ion size influences stress, diffusion, fracture toughness, and electronic properties. Larger isovalent ions (Na + , Ag + , K + ) were exchanged with Li + , with DFT confirming their preference for octahedral 96h sites and a linear relationship between ion size and chemical free expansion coefficient. MD simulations reveal stress and concentration effects on exchange ion diffusivity at elevated temperatures, with Na + and Ag + maintaining favorable mobility while K + showing concentration-dependent clustering. Continuum modeling predicts the range of fracture strength improvements and the required ion exchange concentration profile. It was shown that a 5% surface exchange concentration can induce ∼0.6 GPa of surface compressive stress using Na + and ∼1.0 GPa of surface compressive stress using Ag + . On the other hand, larger ion exchange species may penalize Li + diffusivity by increasing the activation volume and activation energy. Interestingly, Na + has a negligible penalty on Li-ion diffusivity. The room temperature Li + ion diffusivity is reduced by ∼40% with Ag + ion exchange. Electronic band structure analysis shows no size-dependent change in the bandgap, though Ag + introduces localized defect states near the valence band maximum. This study highlights ion size as a key factor in optimizing LLZO properties, offering a framework to improve the solid-state battery performance.

Jagad, Harsh D. [Brown Univ., Providence, RI (Unit↗
DOE OSTI2021

Li 2 S 6 ‐Integrated PEO‐Based Polymer Electrolytes for All‐Solid‐State Lithium‐Metal Batteries

Abstract The integration of Li 2 S 6 within a poly(ethylene oxide) (PEO)‐based polymer electrolyte is demonstrated to improve the polymer electrolyte's ionic conductivity because the strong interplay between O 2− (PEO) and Li + from Li 2 S 6 reduces the crystalline volume within the PEO. The Li/electrolyte interface is stabilized by the in situ formation of an ultra‐thin Li 2 S/Li 2 S 2 layer via the reaction between Li 2 S 6 and lithium metal, which increases the ionic transport at the interface and suppresses lithium dendrite growth. A symmetric Li/Li cell with the Li 2 S 6 ‐integrated composite electrolyte has excellent cyclability and a high critical current density of 0.9 mA cm −2 at 40 °C. Impressive electrochemical performance is demonstrated with all‐solid‐state Li/LiFePO 4 and high‐voltage Li/LiNi 0.8 Mn 0.1 Co 0.1 O 2 cells at 40 °C.

Fang, Ruyi↗
NASA NTRS2003

Mixed Conducting Electrodes for Better AMTEC Cells

Electrode materials that exhibit mixed conductivity (that is, both electronic and ionic conductivity) have been investigated in a continuing effort to improve the performance of the alkali metal thermal-to-electric converter (AMTEC). These electrode materials are intended primarily for use on the cathode side of the sodium-ion-conducting solid electrolyte of a sodium-based AMTEC cell. They may also prove useful in sodium-sulfur batteries, which are under study for use in electric vehicles. An understanding of the roles played by the two types of conduction in the cathode of a sodium-based AMTEC cell is prerequisite to understanding the advantages afforded by these materials. In a sodium-based AMTEC cell, the anode face of an anode/solid-electrolyte/cathode sandwich is exposed to Na vapor at a suitable pressure. Upon making contact with the solid electrolyte on the anode side, Na atoms oxidize to form Na+ ions and electrons. Na+ ions then travel through the electrolyte to the cathode. Na+ ions leave the electrolyte at the cathode/electrolyte interface and are reduced by electrons that have been conducted through an external electrical load from the anode to the cathode. Once the Na+ ions have been reduced to Na atoms, they travel through the cathode to vaporize into a volume where the Na vapor pressure is much lower than it is on the anode side. Thus, the cathode design is subject to competing requirements to be thin enough to allow transport of sodium to the low-pressure side, yet thick enough to afford adequate electronic conductivity. The concept underlying the development of the present mixed conducting electrode materials is the following: The constraint on the thickness of the cathode can be eased by incorporating Na+ -ionconducting material to facilitate transport of sodium through the cathode in ionic form. At the same time, by virtue of the electronically conducting material mixed with the ionically conducting material, reduction of Na+ ions to Na atoms can take place throughout the thickness of the cathode. The net effect is to reduce the diffusion and flow resistance to sodium through the electrode while reducing the electronic resistance by providing shorter conduction paths for electrons. Reduced resistance to both sodium transport and electronic conductivity results in an increase in electric power output.

Ryan, Margaret↗
DOE OSTI2022

Conductivity and Transference Number Determination Protocols for Solid Oxide Cell Materials

To standardize materials and component characterization for next generation hydrogen production and energy generation solid oxide cell (SOC) technologies, test protocols are being established to facilitate comparison across the numerous laboratories and research institutions where SOC development for application in solid oxide fuel cells (SOFCs) and solid oxide electrolyzes cells (SOEC) is conducted. This paper proposes guiding protocols for fundamental electrical properties characterization of SOC materials, including temperature- and oxygen partial pressure (pO 2 )-dependent conductivity measurements, and use of the electromotive force for determining the transference numbers, or contributions of each charge carrier (i.e., ions and electrons), to the total conductivity. The protocol for Archimedes density measurements is also provided as an integral technique to both of these methods.

25 ENERGY STORAGE↗