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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

Balancing solvation: stabilizing lithium metal batteries via optimized cosolvents for ionic-liquid electrolytes

In this study, we examined three cosolvents with distinct solvation capabilities for ionic-liquid electrolytes based on 1-methyl-1-propyl pyrrolidinium bis(fluorosulfonyl)imide (Py13FSI). We demonstrate that 1,1,1-trifluoro-2-(2-(2-(2,2,2-trifluoroethoxy)ethoxy)ethoxy)ethane (FDG) notably enhances the cycle life of Py13FSI-based electrolytes, outperforming 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropylether (TTE) and diglyme (DG). Electrochemical and surface analyses showed that this improvement could be attributed to the formation of a favorable cathode interphase, promoting efficient Li+ transport with reduced overpotential. Spectroscopic techniques (FTIR, Raman, and NMR spectroscopy) and molecular dynamics simulations revealed that cosolvents with varying solvation abilities can influence the solvation structures in Py13FSI-based electrolytes. The mild solvating strength and lithium stability of FDG are key contributors to its effectiveness. Conversely, DG, a strong solvating solvent, destabilized the Py13FSI-DG electrolyte at the lithium metal anode, while TTE, a non-solvating solvent, failed to enhance lithium transport or form a stable cathode interphase. Our findings highlight that balanced solvation exerted by the cosolvents is critical for forming a stable electrolyte–cathode interface, potentially through FSI decomposition. This study offers valuable insights into the development of durable ionic-liquid electrolytes, emphasizing the importance of selecting cosolvents with optimal solvation properties.

Li, Xinlin [Argonne National Laboratory (ANL), Arg↗
DOE OSTI2025

Molecular Interlocking Multidimensional Modulations of Cathode‐Electrolyte Interface for Constructing High Energy Density Quasi‐Solid‐State Batteries

Gel polymers are regarded as a promising candidate electrolyte for lithium-metal quasi-solid-state batteries, primarily due to their high ionic conductivity and solid-liquid synergistic properties. However, challenges such as interfacial side reactions, limitations in Li + transport caused by interfacial issues, and leaching of transition metals from the cathode have yet to be effectively solved. Herein, a novel gel electrolyte modulation strategy based on electrostatic filler assembly is proposed to address the issues of ineffective capacity utilization and inadequate cycling stability of high-energy-density cathode materials in solid-state lithium-ion batteries. It constructs a 3D interpenetrating charge-bridge network that effectively tackles the phase-separation challenge between fillers and electrolytes at the molecular level. Meanwhile, the molecular interlocking structure effectively inhibits the electrolyte erosion. More critically, it optimizes and stabilizes the cathode-electrolyte interface film, which facilitates the conduction of Li + -ions through a size-sieving mechanism. Consequently, this strategy enables effective adaptation across diverse high-energy-density cathode materials with satisfactory capacity performance (170.4 mAh g −1 at 4.5 V/1 C for LiNi 0.6 Co 0.2 Mn 0.2 O 2 and 194.0 mAh g −1 at 4.3 V/1 C for LiNi 0.9 Co 0.08 Mn 0.02 O 2 ). In conclusion, this investigation offers a straightforward and effective reference for addressing the critical challenges of ionic transport and interface stabilization in the design of gel electrolytes.

cathode-electrolyte interface↗
DOE OSTI2022

Single‐Crystal LiNi x Mn y Co 1− x − y O 2 Cathodes for Extreme Fast Charging

Abstract Ni‐rich layered LiNi x Mn y Co 1− x − y O 2 (NMCs, x ≥ 0.8) are poised to be the dominating cathode materials for lithium‐ion batteries for the foreseeable future. Conventional polycrystalline NMCs, however, suffer from severe cracking along the grain boundaries of primary particles and capacity loss under high charge and/or discharge rates, hindering their implementation in fast‐charging electric vehicular (EV) batteries. Single‐crystal (SC) NMCs are attractive alternatives as they eliminate intergranular cracking and allow for grain‐level surface optimization for fast Li transport. In the present study, the authors report synthetic approaches to produce SC LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC811) samples with different morphologies: Oct‐SC811 with predominating (012)‐family surface and Poly‐SC811 with predominating (104)‐family surface. Poly‐SC811, representing the first experimentally synthesized NMC811 single crystals with (104) surface, delivers superior performance even at the ultra‐high rate of 6 C. Through detailed X‐ray analysis and electron microscopy characterization, it is shown that the enhanced performance originates from better chemical and structural stabilities, faster Li + diffusion kinetics, suppressed side reactions with electrolyte, and excellent cracking resistance. These insights provide important design guidelines in the future development of fast‐charging NMC‐type cathode materials.

Lu, Yanying↗
DOE OSTI2021

Developments on two lithium vapor-box linear test-stand experiments

The lithium vapor-box divertor is a possible fusion power exhaust solution.It uses condensation pumping to create a gradient of vapor density in a divertor slot; this should allow a stable detachment front without active feedback.As initial explorations of the concept, two test stands which take the form of three connected cylindrical stainless steel boxes are being developed: one without plasma at PPPL, to test models of lithium evaporation and flow; and one for the linear plasma device Magnum-PSI (at DIFFER in Eindhoven, The Netherlands) to test the ability of a lithium vapor cloud to induce volumetric detachment and redistribute the plasma power.The first experiment uses boxes with diameters of 6 cm, joined by apertures with diameters of 2.2 cm. Up to 1 g of Li is placed in one box, which is heated to up to 600 degrees C. The Li evaporates, then flows to and condenses in the two other, cooler boxes over several minutes. The quantity of Li transported is assessed by weighing the boxes before and after the heating cycle, and is compared to the quantity predicted to flow for the box at its measured temperature using a Direct Simulation Monte Carlo code, SPARTA. With good experimental conditions, the two values agree to within 15%.The experiment on Magnum-PSI is in the conceptual design stage.The design is assessed by simulations using the code B2.5-Eunomia.They show that when the hydrogen-ion plasma beam, with n_e = 4e20 per cubic meter, T_e = 1.5 eV, and r = 1 cm, is passed through a 16 cm long, 12 Pa, 625 degree C Li vapor cloud, the plasma heat flux and pressure on the target are significantly reduced compared to the case without Li.With the Li present, the plasma is cooled by excitation of Li neutrals followed by radiation until it volumetrically recombines, lowering the heat flux from 3.7 MW/m^2 to 0.13 MW/m^2, and the pressure is reduced by 93%, largely by collisions of hydrogen ions with neutral Li.

divertor↗
DOE OSTI2024

A Comprehensive Experimental Study on Microstructure‐Graded Graphite Anodes for Enhancing Fast‐Charging Capability of Lithium‐Ion Batteries

Lithium‐ion batteries with high gravimetric capacity density and improved cycle life performance under fast‐charging conditions are crucial for widespread electric vehicle (EV) adoption. This study investigates how designing graphite anode microstructure, specifically porosity, and particle‐size gradients, improves lithium‐ion (Li + ) transport during fast‐charging conditions. Three‐layered graphite anodes with varying porosity (24%, 36%, 46%) and particle size gradients (3, 5, 10 μm) were compared to a conventional single‐layered electrode in half‐cell configurations. At room temperature and high discharge rate (2C), both gradient structures showed significantly enhanced capacity retention (80% and 67% vs. 50%) compared to the conventional electrode, highlighting the effectiveness of microstructure engineering for fast charging. The study also investigated the temperature's impact on cycle life. After 200 cycles at 2°C and 45°C, all gradient structures demonstrated superior capacity retention (≈80%) compared to the conventional electrode (35%), suggesting the gradients mitigate degradation rate at high temperatures. Electrochemical impedance spectroscopy confirmed superior Li+ diffusion and lower resistivity in gradient electrodes. Simulations explored the influence of gradient profiles on reaction kinetics across the electrode thickness. Overall, this research demonstrates that the fast‐charging capability of graphite electrodes can be greatly enhanced by engineering the electrode microstructure, thereby making EV technology more accessible and appealing.

Ahmadi, Soma↗
DOE OSTI2020

Roll-To-Roll Atomic Layer Deposition of Titania Nanocoating on Thermally Stabilizing Lithium Nickel Cobalt Manganese Oxide Cathodes for Lithium Ion Batteries

Conformal coating of ceramic layers (nm-thick) on Ni-rich layered cathode materials is an effective strategy for improving high-temperature longevity of Li-ion batteries (LIBs). In this work, we develop a roll-to-roll atomic layer deposition (R2R ALD) apparatus for growing uniform nanolayers of TiO 2 . We explore the effect of ALD parameters (temperature: 120–180 °C and line speed: 2–40 mm s –1 ) on the TiO 2 surface coating and subsequently investigate the electrochemical performance of the as-prepared cathodes. The capacity retention of TiO 2 -coated porous electrodes is substantially improved compared to that of the pristine cathode material for high-temperature cycling. Electrochemical impedance spectroscopy confirms that the ALD-TiO 2 coating suppresses the undesired side reactions initiated at the electrode/electrolyte interface, reduces charge transfer resistance, and ultimately facilitates the Li + transport through the composite cathode nanostructure. The robust design of the ALD-TiO 2 cathode material enables high-temperature operation (>55 °C) with enhanced specific capacity, superior rate capability, excellent cyclability, and ultra-high coulombic efficiency within a wide potential window (3.0–4.35 V). Furthermore, the R2R ALD technique developed in this work paves the way for large-scale fabrication of ceramic-coated cathode sheets with a production rate reaching 2.4 m min –1 for a continuous coating operation.

25 ENERGY STORAGE↗
DOE OSTI2020

Potassium Prussian blue-coated Li-rich cathode with enhanced lithium ion storage property

With high specific capacity, the layered Li-rich Mn-based oxide (LRMO) is a promising candidate cathode material for Li-ion batteries. However, the irreversible release of Li-ions during the first charging process, instability of LRMO/electrolyte interface and relatively low ion conductivity of LRMO result in low initial Coulombic efficiency (ICE), poor cycle stability and rate performance, which prohibit its further application. Furthermore, interface engineering via additive coating is expected to effectively address these issues. Herein, we rely on potassium Prussian blue (KPB), a Li + acceptor with good ion conductivity, as a new coating material on LRMO particles. The KPB coating not only forms a protective layer on the surface of LRMO against electrolyte corrosion, but also functions as a host for Li + transport and accommodation, leading to enhanced ion conductivity and ICE of LRMO cathode. Consequently, 2 wt% KPB coated LRMO cathode achieved an initial discharge capacity of up to 281.7 mA h g -1 with an ICE of 85.69% compared to an ICE of 79.52% for the LRMO cathode without coating. The cycling and rate performance are also greatly improved as evidenced by the well maintained capacity of up to 176.8 mA h g -1 after 100 cycles at a current density of 0.5 C, compared to the limited capacity of only 135.3 mA h g -1 for the LRMO cathode without coating. Overall, this work pioneers the use of potassium Prussian blue as additive coating material to enhance performance of LRMO cathode, and we expect it to inspire the battery community with new strategies of material engineering/design toward practical application in high-energy lithium-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Crack‐Free Single‐Crystalline LiNiO 2 for High Energy Density All‐Solid‐State Batteries

Abstract Single‐crystalline layered oxide (LiNi 1‐ x ‐ y Mn x Co y O 2 ) cathodes have been found to exhibit exceptional electrochemical properties when coupled with various inorganic solid electrolytes (ISEs) in all‐solid‐state batteries (ASSBs). Their advantages stem from the robust morphological integrity with the absence of grain boundaries and the high electrochemical oxidative stability. Here, ASSBs featuring single‐crystalline LiNiO 2 (LNO) with the highest Ni content are reported, offering a high theoretical specific capacity of 275 mAh g ‐1 alongside a high average discharge voltage (3.7 V vs Li + /Li). Through a careful investigation, it is demonstrated that micron‐sized single‐crystalline LNO (µSC‐LNO) composite cathodes with a halide ISE exhibit a high initial discharge capacity of 205 mAh g ‐1 with an outstanding cycle performance over 200 cycles in room‐temperature ASSBs. The significance of engineering parameters is emphasized, such as particle size and specific density, in promoting a homogeneous and fast Li + transport within the composite cathodes. Furthermore, the formation of undesirable interphase between the halide ISE in the cathode and sulfide ISE separator is elucidated, which may be a critical factor impeding long‐term cyclability of ASSBs. This work provides insights into the design of composite cathodes for high‐energy‐density ASSBs.

Chemistry↗
DOE OSTI2022

Tailored Solvation and Interface Structures by Tetrahydrofuran-Derived Electrolyte Facilitates Ultralow Temperature Lithium Metal Battery Operations

Ineffectiveness of Li-ion batteries (LIBs) in cold climates hinders electronics to work in various conditions including frigid environments, despite high demands. Given that intrinsic properties of LIB materials cause this problem, optimized cell chemistries ultimately are required for low-temperature usage. In this study, Li-metal batteries (LMBs) composed of a Li-metal anode (LMA) stabilized by a localized high-concentration electrolyte (LHCE) are found to significantly enhance low-temperature performance. The LHCE allows the LMA to have compact and regular deposition and excellent plating/stripping efficiency at sub-zero temperatures. The LHCE produces an inorganic-rich solid-electrolyte interphase with larger amounts of Li 2 O/LiF interfaces, dominance of ion aggregates in Li + solvation, and enhanced Li + transport, which can greatly improve the LMA stability. LMB full cells based on LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes with the tailored electrolyte show high retentions of 75 and 64 % at -20 and -40 °C, respectively. Furthermore, the LMB configuration retains its charge-discharge capability even at -60 °C.

25 ENERGY STORAGE↗
DOE OSTI2023

Silver-carbon interlayers in anode-free solid-state lithium metal batteries: Current development, interfacial issues, and instability challenges

As an interlayer between the anode and the electrolyte of the all-solid-state lithium metal batteries (ASSLMBs), the silver-carbon (Ag-C) nanocomposite has been reported to significantly increase the energy density and cycle rate of solid-state lithium metal batteries. Ag-C interlayers serve as mixed ionic-electronic conductor that conducts both Li+ ions and electrons and lithium storage capacity. Unfortunately, it was unclear how the Ag-C interlayer regulated lithium plating and stripping. Moreover, the structural and chemical instabilities between the interlayer and the electrolyte, within the interlayer, or beneath the interlayer on lithium substrate are likely to cause cell failure. In this review, we discuss interfacial issues and summarize recent progress in solution strategies for ASSLMBs, with a specific focus on the use of a silver-carbon (Ag-C) nanocomposite interlayer in anode-free setups. Based on the Li transport kinetics among the Ag-C interlayers, the interfacial configurations of Ag-C interlayers are classified as either exterior or internal. Furthermore, the review concludes with a discussion of the perspectives and future prospects, allowing for the improvement of interlayer techniques for solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Atomic defects, functional groups and properties in MXenes

MXenes, a new family of functional two-dimensional (2D) materials, have shown great potential for an extensive variety of applications within the last decade. Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties. In this review, we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes, and how to control them to directly influence various properties ( e.g ., electron transport, Li + adsorption, hydrogen evolution reaction (HER) activity, and magnetism) of 2D MXenes materials. Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed. The review thus provides perspectives on property optimization through atomic defect engineering, and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Computational modeling of coupled mechanical damage and electrochemistry in ternary oxide composite electrodes

Performance degradation of ternary layered oxide cathodes largely originates from their loss of structural integrity in cyclic usage. Mechanical damage, such as intergranular fracture of the active particles, is not only a mechanical cleavage process but also interferes with electrochemical kinetics such as infiltration of liquid electrolyte, surface corrosion of the constituent primary particles, and may eventually isolate the primary grains from the electron conducting network. Here, in this work, we develop a computational framework that integrates electrochemistry of a LiNi x Mn y Co 1−x−y O 2 (NMC) composite cathode with mechanical damage of the active particles. To fully examine the intricate chemomechanical behavior of the electrode, we evaluate the effects of the anisotropic material properties, the influence of mechanical potential on Li transport, and the concurrent intergranular fracture and electrolyte penetration along the grain boundaries upon multiple cycles. Electrolyte infiltration benefits capacity retention but aggravates further mechanical damage by corrosion. Structural failure mostly occurs in the first charging due to the anisotropic mechanical strain between the primary grains, while the resulting damage remains stable in the later few cycles. The results are consistent with experimental observations and the integration of electrochemistry and mechanical failure enables a step further understanding of the complex mechanism of battery degradation.

Battery degradation↗
DOE OSTI2025

Fast-Charging Li-Ion Battery Enabled by an Acetonitrile-Based Electrolyte

Fast charging remains a critical challenge for current-generation lithium-ion batteries (LIBs), particularly in electric vehicle applications. Here, in this study, we present a highly conductive electrolyte formulation based on a ternary solvent system consisting of acetonitrile (AN), fluoroethylene carbonate (FEC), and ethylene carbonate (EC), combined with a tailored additive, lithium difluoro­(oxalato)­borate (LiDFOB). This electrolyte demonstrates significantly enhanced ionic conductivity and a higher Li + transference number, enabling accelerated Li + transport kinetics. The synergistic effect of the solvents and the additive promotes the formation of a robust, low-resistance, inorganic-rich solid-electrolyte-interphase (SEI) that effectively passivates the graphite surface and suppresses AN decomposition. As a result, the electrolyte substantially reduces internal cell resistance and overpotential, both of which are critical for reliable fast charging. These findings highlight the essential role of rational electrolyte design in addressing the limitations of fast-charging LIBs.

Wu, Dezhen [Argonne National Laboratory (ANL), Arg↗
DOE OSTI2021

Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes

A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. In this work, we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li + transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Electron leakage through heterogeneous LiF on lithium–metal battery anodes

The solid–electrolyte interphase (SEI) that forms on lithium ion battery (LIB) anodes prevents degradation-causing transfer of electrons to the electrolyte. Grain boundaries (GBs) between different SEI components, like LiF, have been suggested to accelerate Li+ transport. However, using the non-equilibrium Green's function technique with density functional theory (NEGF-DFT), we find that GBs enhance electron tunneling in thin LiF films by 1–2 orders of magnitude, depending on the bias. Extrapolating to thicker films using the Wentzel–Kramers–Brillouin (WKB) method emphasizes that safer batteries require passivation of GBs in the SEI.

25 ENERGY STORAGE↗
DOE OSTI2021

3D Printed, Low Tortuosity Garnet Framework For Beyond 500 Wh/kg Batteries

In this project, we developed LLZO garnet ink recipes and processes for 3D-printing highly ordered ionically conductive garnet porous structures on dense garnet separators. Using this technique, we are able to fabricate controlled architecture LLZO garnet solid-state electrolyte (SSE) trilayers for application in solid-state lithium batteries. The trilayer comprises a thin dense center layer sandwiched between a 3D-printed patterned porous layer and a random porous layer. The dense layer functions as the ionic separator between the anode and cathode. The random porous layer hosts the lithium-metal anode and provides the structural support. The 3D-printed SSE patterned porous layer hosts the cathode, providing continuous, low tortuosity pathways for fast 3D Li+ transport through the cell while increasing the electrode/electrolyte interface area to decrease the interfacial resistance. Compared to the random porous structure, this ordered patterned structure possesses more vacant space for higher cathode loading without sacrificing ionically conducting capability, thus potentially greatly increasing the cell energy density. For demonstration purposes, we developed two patterns for the 3D-printed porous layer: grids and columns, for hosting sulfur and NMC cathode, respectively. The corresponding two types of cells were fabricated and tested, and have demonstrated achievement of theoretical discharge capacity without cathode calendaring. In addition, we developed a fundamental solid-state ionic and electronic transport model to optimize the 3D-printed structures for maximum energy and power density. The model was validated by experiment and provides the critical design criteria for achieving the >500 Wh/kg energy goal as function of C-rate.

25 ENERGY STORAGE↗
DOE OSTI2020

A Micelle Electrolyte Enabled by Fluorinated Ether Additives for Polysulfide Suppression and Li Metal Stabilization in Li-S Battery

The Li-S battery is a promising next-generation technology due to its high theoretical energy density (2600 Wh kg -1 ) and low active material cost. However, poor cycling stability and coulombic efficiency caused by polysulfide dissolution have proven to be major obstacles for a practical Li-S battery implementation. In this work, we develop a novel strategy to suppress polysulfide dissolution using hydrofluoroethers (HFEs) with bi-functional, amphiphlic surfactant-like design: a polar lithiophilic "head" attached to a fluorinated lithiophobic "tail." A unique solvation mechanism is proposed for these solvents whereby dissociated lithium ions are readily coordinated with lithiophilic "head" to induce self-assembly into micelle-like complex structures. Complex formation is verified experimentally by changing the additive structure and concentration using small angle X-ray scattering (SAXS). These HFE-based electrolytes are found to prevent polysulfide dissolution and to have excellent chemical compatibility with lithium metal: Li||Cu stripping/plating tests reveal high coulombic efficiency (>99.5%), modest polarization, and smooth surface morphology of the uniformly deposited lithium. Li-S cells are demonstrated with 1395 mAh g-1 initial capacity and 71.9% retention over 100 cycles at >99.5% efficiency-evidence that the micelle structure of the amphiphilic additives in HFEs can prohibit polysulfide dissolution while enabling facile Li + transport and anode passivation.

25 ENERGY STORAGE↗
NASA NTRS1985

Development of a lithium secondary battery separator

A nonporous membrane based on the polymerization of 2,3-dihydrofuran followed by crosslinking in situ was prepared. The material is compatible with rechargeable Li battery components and, when swollen with an appropriate solvent such as tetrahydrofuran, exhibits separator resistance and Li transport equivalent to Celgard.

Moore, J. A.↗