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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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192 records · Page 2

Interface Evolutionand Long-Term Performance of NegativeCarbon Fiber Structural Electrodes

Abstract Laminated structural batteries present a transformative solution to reducing weight constraints in electric vehicles. These structural batteries are based on a multifunctional material that incorporates an energy storage function within a carbon fiber-reinforced polymer. Despite the potential of this technology, the intricate morphology of fiber–matrix or electrode–electrolyte interfaces and the impact of long-term cycling at low current rates (C-rates) on these interfaces remain insufficiently understood. This study addresses these critical knowledge gaps by examining the influence of matrix composition on the long-term electrochemical performance of structural battery electrodes and exploring advanced techniques to investigate carbon fiber–matrix interfaces. Localized imaging and X-ray scattering techniques were used to characterize morphological changes at the electrode–electrolyte interfaces by analyzing negative structural electrodes. The findings revealed that the matrix composition influences long-term electrochemical behavior and fiber–matrix interface formation. While the intrinsic properties of carbon fibers largely remain unaffected by long-term cycling, cycling promotes debonding at fiber–matrix interfaces. Nonetheless, residual regions of adhesion persist, underscoring the potential for preserving multifunctionality even under prolonged cycling conditions. These insights advance the understanding of interface dynamics, which is critical for optimizing structural battery technologies.

Chemistry

Development of Electrolytes under Lean Condition in Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries stand out as one of the promising candidates for next-generation electrochemical energy storage technologies. A key requirement to realize high-specific-energy Li–S batteries is to implement low amount of electrolyte, often characterized by the electrolyte/sulfur (E/S) ratio. Low E/S ratio aggravates the known challenges for Li–S batteries and introduces new ones originated from the high concentration of polysulfides in limited electrolyte reservoir. Here, in this review, the connections between the fundamental properties of electrolytes and the electrochemical/chemical reactions in Li–S batteries under lean electrolyte condition are elucidated. The emphasis is on how the solvating properties of the electrolyte affect the fate of polysulfides. Built upon the mechanistic analysis, different strategies to design lean electrolytes to improve the overall process of Li–S reactions and Li anode protection are discussed.

25 ENERGY STORAGE

Advanced LiFSI-LiPF6 Electrolyte for Wide-Temperature and Thermally Stable Lithium-Ion Batteries

A new optimized LiFSI–LiPF6 dual-salt controlled-solvation electrolyte (E-DS) is demonstrated to enable practical graphite||LiNi0.8Mn0.1Co0.1O2 cells (˜4.0 mAh cm?²) to achieve exceptional performance and safety under extreme conditions. By optimizing anion coordination with the smaller, more dissociating FSI? anion, the E-DS forms ultrathin, dense, and inorganic-rich electrode/electrolyte interphases that dramatically suppress solvent decomposition, transition-metal dissolution, and surface reconstruction compared to the conventional LiPF6/carbonate electrolyte. Consequently, E-DS cells deliver >78% capacity retention after 300 cycles at 60 °C, retain fast discharging capacity at 30 °C, and operate effectively at -20 °C. Most strikingly, fully charged full cells with E-DS, even under overcharging to 4.8 V, show a lower heat evolution in stable formulations — transforming a traditionally unstable high-voltage/high-temperature configuration into an intrinsically safe state. This work establishes a new benchmark for carbonate-containing electrolytes, simultaneously achieving high energy density, fast-discharging capability, wide-temperature operation (-20 to 60 °C), and outstanding thermal safety in nickel-rich lithium-ion batteries.

electrode/electrolyte interphase

Heat Transfer Fluids as Co‐Diluents in Localized High‐Concentration Electrolytes for High‐Rate Lithium Metal Batteries With Enhanced Safety

Localized high-concentration electrolytes (LHCEs) have been identified as promising electrolyte formulations for lithium metal batteries, due to their effective interphase formation and promotion of compact Li deposition, yet their practical implementation is often limited by reduced ion transport kinetics. In this study, two industrially established fluorinated ethers are identified for the first time in battery research as effective co-diluents as they combine a broad electrochemical stability window with a low viscosity and intrinsic non-flammability. Incorporating these components, commonly used as heat transfer fluids, yields safer, less flammable electrolyte formulations with enhanced ion mobilities. In particular, the ternary co-diluent formulation shows improved ion mobility by reducing the electrolyte's viscosity while limiting excessive ion clustering. Based on the improved electrolyte transport kinetics, lower overvoltages and higher Coulombic efficiencies at current densities ≥ 1 mA cm −2 are achieved with the ternary co-diluent blend, resulting in markedly extended cycle life in an application-oriented zero-excess pouch cell compared with the baseline system. Complementary electrochemical and ex situ analysis of harvested electrodes at moderate current densities reveals no discernible differences in interphase morphology and composition, suggesting enhanced ion mobility as the primary cause of the improved high-rate performance.

electrolyte diluent

Investigation Into LiCl-LiF+Li 2 O as a Low Temperature Electrolyte in Direct Electrolytic Reduction of UO 2

Direct electrolytic reduction (DER) of UO 2 in a binary LiCl-Li2O (1–3 wt%) at 650 °C has been widely reported. The process temperature can be reduced to 550 °C in theory by using a near eutectic ternary LiCl-LiF+Li 2O (∼2 wt%) electrolyte, which will result in substantial reduction in rate of salt vaporization. The feasibility of using the ternary electrolyte for the process was tested via material compatibility testing, electrochemical polarization testing, and controlled potential or current DER experiments. MgO, Pt, and 625 nickel samples were each contacted with the ternary salt for 168 h. Negligible changes to dimensions and mass of the samples were measured, and concentrations of corrosion products in the salt were 102 ppm or less. O2−oxidation was observed to occur at a lower potential than Cl-or F-on a Pt anode. DER of UO2was performed in six trials. Process variables included type of reference electrode, electrochemical control method, type of cathode basket, and electrolyte composition. UO 2conversion ranged from 28.2 to 99.9 % , and current efficiency ranged from 38 to 52%. Overall, results indicate that the use of the ternary salt is feasible for DER.

36 MATERIALS SCIENCE

Methodology of Atomic Force Microscopy Visualization of Electrode–Electrolyte Interfaces

Electrochemical atomic force microscopy (EC-AFM) provides unprecedented insights into the microstructure of electrode–electrolyte interfaces during electrochemical reactions. However, performing EC-AFM measurements has many challenges, for example, drift, contamination, and probe degradation. We present solutions to these experimental issues through electrochemical cell design and carefully chosen experimental parameters. The possibility that the probes can react with the interface during scanning, generating false-positive electrochemical dynamics, is discussed as an example of the challenge of high-fidelity EC-AFM measurement. Here, we demonstrate this effect in highly ordered pyrolytic graphite and show that we could use electrochemical control of the AFM probe to enable high-fidelity in situ AFM visualization of solid–liquid interfaces during electrochemical reactions.

Electrochemical cells

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

Decoupling Failure Pathways in Li-O 2 Cells Operated Under Lean Electrolyte Conditions

The operation of lithium-oxygen (Li-O 2 ) batteries under lean electrolyte conditions offers higher energy density but leads to rapid degradation and short cycle life. Although cathode passivation and electrolyte decomposition occur in all regimes, we show that under lean electrolyte conditions, failure is primarily driven by progressive electrolyte consumption at the lithium/solid electrolyte interphase (SEI), rather than by irreversible cathode passivation. Poor wetting of the lithium surface results in heterogeneous SEI growth and high local current densities, which accelerate electrolyte loss and cell failure. Strategies aimed at improving interfacial stability, including optimized wetting and SEI forming additives, significantly extend cycle life without compromising energy density. Our results establish anode-electrolyte interactions as the dominant degradation mechanism under lean electrolyte conditions, and emphasize the need to engineer a stable Li/SEI interface for long-lasting Li-O 2 batteries.

Córdoba, Daniel [Argonne National Laboratory (ANL)

Polymer grafted aramid nanofiber reinforces immiscible waste polypropylene/poly(ethylene terephthalate)

Polypropylene (PP) and poly(ethylene terephthalate) (PET) are plastics commonly used for packaging because of their excellent barrier and mechanical properties. The properties of these plastics are often diminished after mechanical recycling, inevitably causing down-cycling. Furthermore, this problem is exacerbated when different kinds of polymers mix. Aramid nanofibers have the potential to improve the mechanical properties of polymers due to their excellent mechanical properties but their poor dispersion in polymers is a challenge. Grafting polymers onto nanofibers can help address this challenge. In this work, different loading levels (1%, 2%, and 5%) of polymer grafted aramid nanofibers (ANFs) are blended with waste PP/PET (90/10), simulating a PP waste stream containing traces of PET contaminants. Scanning electronic microscopy, rheology, and differential scanning calorimetry results show the affinity of PP functionalized aramid nanofibers (PP_ANF) towards the PP matrix. At 1 wt% of the nanofiber, the size of the PET droplets in the PP matrix of the PP_ANF blend range from 0.2 to 2.0 μm while that of unmodified ANF and PET_ANF blends are in the range of 0.1–6.2 and 0.5–7.4 μm, respectively. In summary, polymer grafted ANFs have the tendency of improving properties of its like polymers due to similarity in the grafting polymer and the polymer matrix.

36 MATERIALS SCIENCE

Interlayer Design for Halide Electrolytes in All‐Solid‐State Lithium Metal Batteries

Abstract All‐solid‐state lithium‐metal batteries (ASSLMBs) are promising for transportation electrification due to their superior safety and high energy density. Lithium halide electrolytes provide excellent processing flexibility, high ionic conductivity, and anodic stability (>4.1 V), making them highly compatible with high‐voltage cathodes, surpassing sulfide electrolytes (<2.1 V). Nevertheless, halide electrolytes suffer from low cathodic stability and form an electronically conductive interphase with lithium, resulting in a critical current density (CCD) of nearly zero. Herein, Li 3 YbCl 6 electrolytes are synthesized that are kinetically stable with lithium by forming an electronic insulating solid electrolyte interphase. Guided by critical overpotential criteria, a PI 3 interlayer is designed that transforms into Li 6 PI 3 upon contact with lithium, substantially reducing the interfacial resistance of Li 3 YbCl 6 against lithium to 34 Ω and achieving a high critical overpotential of 114 mV. By substituting Yb with Lu, Li 3 LuCl 6 electrolytes with Li 6 PI 3 interlayers reach a CCD of 1.0 mA cm −2 at a capacity of 1.0 mAh cm −2 , comparable to sulfide electrolytes but with higher oxidation stability. Additionally, Li 6 PI 3 enables stable cycling of Li//Li cells with Li 3 LuCl 6 electrolytes at 0.5 mA cm −2 for 400 cycles and maintains 86.5% capacity in Li//LiCoO 2 cells after 220 cycles at 30 °C, paving the way for high‐performance ASSLMBs.

Chemistry