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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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Li-Rich and Halide-Deficient Argyrodite Fast Ion Conductors

Here, we report on a new family of halide-deficient and Li-rich argyrodite fast-ion conductors, Li 6+x PS 5+x (Cl/Br/I) 1–x (0 ≤ x ≤ 0.85). Exploration of the influence of aliovalent anion substitution in Li 6 PS 5 X (X = Cl, Br, I)–using a combination of high-resolution powder neutron diffraction and electrochemical impedance spectroscopy–reveals that aliovalent anion substitution induces higher Li-ion concentration and Li site disorder, and creates S 2– /I – anion site disorder on the 4a site. In the series Li 6+x PS 5+x I 1–x (0 ≤ x ≤ 0.4), the resulting conductivity for Li 6.4 PS 5.4 I 0.6 (0.13 mS·cm –1 ) represents almost a 100-fold increase over that of the parent phase, Li 6 PS 5 I (0.0033 mS·cm –1 ), and establishes one of the first fast-ion conducting argyrodite thiophosphate iodides. For Cl-argyrodites, the ionic conductivity decreases a little with lower halide-content but ionic conductivity for the Br-argyrodites is almost unchanged. Overall, all Cl/Br-argyrodites Li 6 +xPS 5+x (Cl/Br) 1–x (0 ≤ x ≤ 0.75) with a low halide content exhibit surprisingly high ionic conductivities > 1 mS·cm –1 despite a very low degree of sulfur/halogen anion site disorder. Our findings highlight the importance of attaining a disordered Li-ion sublattice and sulfur/halogen anion site disorder (anionic charge homogeneity) in argyrodites, where Li ions occupy high energy sites and activate concerted ion migration that drives the ionic conductivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Enhanced Conductivity via Homopolymer-Rich Pathways in Block Polymer-Blended Electrolytes

The optimization of ionic conductivity and lithium-ion battery stability can be achieved by independently tuning the ion transport and mechanical robustness of block polymer (BP) electrolytes. However, the ionic conductivity of BP electrolytes is inherently limited by the covalent attachment of the ionically conductive block to the mechanically robust block, among other factors. Herein, the BP electrolyte polystyrene-block-poly(oligo-oxyethylene methacrylate) [PS-b-POEM] was blended with POEM homopolymers of varying molecular weights. The incorporation of a higher molecular weight homopolymer additive (α > 1 state) promoted a “dry brush-like” homopolymer distribution within the BP self-assembly and led to higher lithium salt concentrations in the more mobile homopolymer-rich region, increasing overall ionic conductivity relative to the “wet brush-like” (α < 1 state) and unblended composites, where α is the molecular weight ratio between the POEM homopolymer and the POEM block in the copolymer. Here, neutron and X-ray reflectometry (NR and XRR, respectively) provided additional details on the lithium salt and polymer distributions. From XRR, the α > 1 blends showed increased interfacial widths in comparison to their BP (unblended) or α < 1 counterparts because of the more central distribution of the homopolymer. This result, paired with NR data that suggested even salt concentrations across the POEM domains, implied that there was a higher salt concentration in the homopolymer POEM-rich regions in the dry brush blend than in the wet brush blend. Furthermore, using 7 Li solid-state nuclear magnetic resonance spectroscopy, we found a temperature corresponding to a transition in lithium mobility (T Li mobility ) that was a function of blend type. T Li mobility was found to be 39 °C above T g in all cases. Interestingly, the ionic conductivity of the blended BPs was highest in the α > 1 composites, even though these composites had higher T g s than the α < 1 composites, demonstrating that homopolymer-rich conducting pathways formed in the α > 1 assemblies had a larger influence on conductivity than the greater lithium ion mobility in the α < 1 blends.

25 ENERGY STORAGE↗
DOE OSTI2023

Interface-enhanced conductivities in surfactant-mediated, solution-grown ionic crystalline complexes

Renewable energy is increasingly relying on optimized electrolytes and interfaces. In this work, Tween 20 and sodium chloride are selected as a model system to reveal the effects of surfactants on salt crystallization in the context of ionic conductivity and interface optimization. At a varied crystallization speed and mix ratio, it is demonstrated that the resultant solution-grown ionic crystalline complexes can achieve a highly tunable ion transport with a controllable crystalline interface. X-ray diffraction results rule out the possibility of polymorphism in the NaCl/Tween 20 systems, which further supports the importance of an optimized crystalline network for optimizing permittivity or ionic conductivity. Raman mapping and machine learning techniques are used to perform semantic segmentation on highly heterogeneous NaCl/Tween 20 complexes. Furthermore, FTIR measurements demonstrate that inter- and intra-molecular interactions play critical roles in the formation of these crystals. This work lays a foundation toward future optimization of such complex ion systems for a specific salt or crystallization modifier in energy storage or ion transport applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Design principles for NASICON super-ionic conductors

Na Super Ionic Conductor (NASICON) materials are an important class of solid-state electrolytes owing to their high ionic conductivity and superior chemical and electrochemical stability. In this paper, we combine first-principles calculations, experimental synthesis and testing, and natural language-driven text-mined historical data on NASICON ionic conductivity to achieve clear insights into how chemical composition influences the Na-ion conductivity. These insights, together with a high-throughput first-principles analysis of the compositional space over which NASICONs are expected to be stable, lead to the successful synthesis and electrochemical investigation of several new NASICONs solid-state conductors. Among these, a high ionic conductivity of 1.2 mS cm ₋1 could be achieved at 25 °C. We find that the ionic conductivity increases with average metal size up to a certain value and that the substitution of PO 4 polyanions by SiO 4 also enhances the ionic conductivity. While optimal ionic conductivity is found near a Na content of 3 per formula unit, the exact optimum depends on other compositional variables. Surprisingly, the Na content enhances the ionic conductivity mostly through its effect on the activation barrier, rather than through the carrier concentration. These deconvoluted design criteria may provide guidelines for the design of optimized NASICON conductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Room-temperature cycling of metal fluoride electrodes: Liquid electrolytes for high-energy fluoride ion cells

Fluoride ion batteries are potential “next-generation” electrochemical storage devices that offer high energy density. At present, such batteries are limited to operation at high temperatures because suitable fluoride ion–conducting electrolytes are known only in the solid state. We report a liquid fluoride ion–conducting electrolyte with high ionic conductivity, wide operating voltage, and robust chemical stability based on dry tetraalkylammonium fluoride salts in ether solvents. Pairing this liquid electrolyte with a copper–lanthanum trifluoride (Cu@LaF 3 ) core-shell cathode, we demonstrate reversible fluorination and defluorination reactions in a fluoride ion electrochemical cell cycled at room temperature. Fluoride ion–mediated electrochemistry offers a pathway toward developing capacities beyond that of lithium ion technology.

Davis, Victoria K.↗
DOE OSTI2014

Synergistic Effects of Mixing Sulfone and Ionic Liquid as Safe Electrolytes for Lithium Sulfur Batteries

Here we report a strategy of mixing both the ionic liquid and sulfone with synergistic effects of reducing viscosity, increasing ionic conductivity, reducing the polysulfide dissolution, and improving the safety. The mixtures of the ionic liquids and sulfones also show distinctly different physicochemical properties, including the thermal properties and crystallization behavior. Using these electrolytes, lithium sulfur batteries assembled with lithium and mesoporous carbon composites show a reversible specific capacity of 1265 mAh g-1 (second cycle) by using 40% 1.0 M LiTFSI in MPPY∙TFSI with 60% 1.0 M LiTFSI in MIPS in the first cycle. This capacity is slightly lower than what was obtained in the pure 1.0 M LiTFSI in the sulfone electrolytes; however, it exhibits an excellent cycling stability and remains as high as 655 mAh g-1 even after 50 cycles. Our strategy provides a method to alleviate the polysulfide dissolution and redox shuttle phenomenon, with an improved ionic conductivity at the same time.

electrochemistry↗
DOE OSTI2016

Communication: Influence of nanophase segregation on ion transport in room temperature ionic liquids

In this paper, we report measurements of the ionic conductivity, shear viscosity, and structural dynamics in a homologous series of quaternary ammonium ionic liquids (ILs) and a prototypical imidazolium-based IL over a wide range of temperatures down to the glass transition. We find that the ionic conductivity of these materials generally decreases, while the shear viscosity correspondingly increases, with increasing volume fraction of aliphatic side groups. Upon crossing an aliphatic volume fraction of ~0.40, we observe a sharp, order-of-magnitude decrease in ionic conductivity and enhancement of viscosity, which coincides with the presence of long-lived, nanometer-sized alkyl aggregates. These strong changes in dynamics are not mirrored in the ionicity of these ILs, which decreases nearly linearly with aliphatic volume fraction. Finally, our results demonstrate that nanophase segregation in neat ILs strongly reduces ionic conductivity primarily due to an aggregation-induced suppression of dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Using Data-Science Approaches to Unravel Insights for Enhanced Transport of Lithium Ions in Single-Ion Conducting Polymer Electrolytes

Solid polymer electrolytes have yet to achieve the desired ionic conductivity (>1 mS/cm) near room temperature required for many applications. This target implies the need to reduce the effective energy barriers for ion transport in polymer electrolytes to around 20 kJ/mol. In this work, we combine information extracted from existing experimental results with theoretical calculations to provide insights into ion transport in single-ion conductors (SICs) with a focus on lithium ion SICs. Through the analysis of temperature-dependent ionic conductivity data obtained from the literature, we evaluate different methods of extracting energy barriers for lithium transport. The traditional Arrhenius fit to the temperature-dependent ionic conductivity data indicates that the Meyer–Neldel rule holds for SICs. However, the values of the fitting parameters remain unphysical. Our modified approach based on recent work (Macromolecules 2023, 56, 15, 6051), which incorporates a fixed pre-exponential factor, reveals that the energy barriers exhibit temperature dependence over a wide range of temperatures. Using this approach, we identify anions leading to the energy barriers <30 kJ/mol, which include trifluoromethane sulfonimide (TFSI), fluoromethane sulfonimide (FSI), and boron-based organic anions. In our efforts to design the next generation of anions, which can exhibit the energy barriers <20 kJ/mol, we have performed density functional theory (DFT) based calculations to connect the chemical structures of boron-based anions via the binding energy of cation (lithium)-anion pairs with the experimentally derived effective energy barriers for ion hopping. Not only have we identified a correlation between the binding energy and the energy barriers, but we also propose a strategy to design new boron-based anions by using the correlation. This combined approach involving experiments and theoretical calculations is capable of facilitating the identification of promising new anions, which can exhibit ionic conductivity >1 mS/cm near room temperature, thereby expediting the development of novel superionic single-ion conducting polymer electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

The effects of lithium doping level on the structural, electrical properties of Li{sup +}-doped BPO{sub 4} solid electrolyte

Graphical abstract: - Highlights: • Better ionic conductivities when 0.05 ≤ x ≤ 0.13. • V{sup ‴}{sub B}+3Li{sub i} model was preferred. • Grain size, lattice strain and Li{sup +}conductivity are closely related. - Abstract: A series of lithium ion conducting solid electrolytes Li{sub x}B{sub 1−x/3}PO{sub 4}(x = 0.01, 0.05, 0.09, 0.13, 0.17, 0.20) is synthesized by a soft-chemistry route. FTIR and XRD measurements reveal that the electrolyte is pure phase of tetragonal structure. AC-impedance spectroscopy (AC-IS) at room temperature shows that Li{sub x}B{sub 1−x/3}PO{sub 4} exhibits higher ionic conductivities in the range 0.05 ≤ x ≤ 0.13, beyond which, the ionic conductivities decrease quickly. Maximum ionic conductivity of the Li{sub x}B{sub 1−x/3}PO{sub 4} reaches 3.35 × 10{sup −5} S cm{sup −1} at room temperature for x = 0.05. Direct current polarizing (DCP) measurement indicates that the decomposition voltage for the solid electrolyte reaches up to 3.7 V. Micro-structure parameters of synthesized Li{sub x}B{sub 1−x/3}PO{sub 4} samples are calculated by Rietveld refinement of X-ray diffraction spectra. The unit-cell parameters, lattice strain, crystal grain size and ionic conductivities of the samples are correlated with the lithium ion doping level x.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Defect-driven anomalous transport in fast-ion conducting solid electrolytes

We report solid-state ionic conduction is a key enabler of electrochemical energy storage and conversion. The mechanistic connections between material processing, defect chemistry, transport dynamics, and practical performance are of considerable importance, but remain incomplete. Here, inspired by studies of fluids and biophysical systems, we re-examine anomalous diffusion in the iconic two-dimensional fast-ion conductors, the β- and β"-aluminas. Using large-scale simulations, we reproduce the frequency dependence of alternating-current ionic conductivity data. We show how the distribution of charge-compensating defects, modulated by processing, drives static and dynamic disorder, which lead to persistent sub-diffusive ion transport at macroscopic timescales. We deconvolute the effects of repulsions between mobile ions, the attraction between the mobile ions and charge-compensating defects, and geometric crowding on ionic conductivity. Our quantitative framework based on these model solid electrolytes connects their atomistic defect chemistry to macroscopic performance with minimal assumptions and enables mechanism-driven 'atoms-to-device' optimization of fast-ion conductors.

25 ENERGY STORAGE↗
DOE OSTI2016

Poly(vinylidene fluoride-hexafluoropropylene) polymer electrolyte for paper-based and flexible battery applications

Paper-based batteries represent a new frontier in battery technology. However, low-flexibility and poor ionic conductivity of solid electrolytes have been major impediments in achieving practical mechanically flexible batteries. This work discuss new highly ionic conductive polymer gel electrolytes for paper-based battery applications. In this paper, we present a poly(vinylidene fluoride-hexafluoropropylene) (PVDH-HFP) porous membrane electrolyte enhanced with lithium bis(trifluoromethane sulphone)imide (LiTFSI) and lithium aluminum titanium phosphate (LATP), with an ionic conductivity of 2.1 × 10{sup −3} S cm{sup −1}. Combining ceramic (LATP) with the gel structure of PVDF-HFP and LiTFSI ionic liquid harnesses benefits of ceramic and gel electrolytes in providing flexible electrolytes with a high ionic conductivity. In a flexibility test experiment, bending the polymer electrolyte at 90° for 20 times resulted in 14% decrease in ionic conductivity. Efforts to further improving the flexibility of the presented electrolyte are ongoing. Using this electrolyte, full-cell batteries with lithium titanium oxide (LTO) and lithium cobalt oxide (LCO) electrodes and (i) standard metallic current collectors and (ii) paper-based current collectors were fabricated and tested. The achieved specific capacities were (i) 123 mAh g{sup −1} for standard metallic current collectors and (ii) 99.5 mAh g{sup −1} for paper-based current collectors. Thus, the presented electrolyte has potential to become a viable candidate in paper-based and flexible battery applications. Fabrication methods, experimental procedures, and test results for the polymer gel electrolyte and batteries are presented and discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2014

Computational and Experimental Investigation of Li-doped Ionic Liquid Electrolytes: [pyr14][tfsi], [pyr13][fsi], and [EMIM][BF4]

We employ molecular dynamics (MD) simulation and experiment to investigate the structure, thermodynamics, and transport of N-methyl-N-butylpyrrolidinium bis(trifluoromethylsufonyl)imide ([pyr14][TFSI]), N -methyl-N-propylpyrrolidinium bis(fluorosufonyl)imide ([pyr13][FSI]), and 1-ethyl-3-methylimidazolium boron tetrafluoride ([EMIM][BF4]), as a function of Li-salt mole fraction (0.05 xLi+ 0.33) and temperature (298 K T 393 K). Structurally, Li+ is shown to be solvated by three anion neigh- bors in [pyr14][TFSI] and four anion neighbors in both [pyr13][FSI] and [EMIM][BF4], and at all levels of xLi+ we find the presence of lithium aggregates. Pulsed field gradient spin-echo NMR measurements of diffusion and electrochemical impedance spectroscopy measurements of ionic conductivity are made for the neat ionic liquids as well as 0.5 molal solutions of Li-salt in the ionic liquids. Bulk ionic liquid properties (density, diffusion, viscosity, and ionic conductivity) are obtained with MD and show excellent agreement with experiment. While the diffusion exhibits a systematic decrease with increasing xLi+, the contribution of Li+ to ionic conductivity increases until reach- ing a saturation doping level of xLi+ 0.10. Comparatively, the Li+ conductivity of [pyr14][TFSI] is an order of magnitude lower than that of the other liquids, which range between 0.1-0.3 mScm. Our transport results also demonstrate the necessity of long MD simulation runs ( 200 ns) required to converge transport properties at room T. The differences in Li+ transport are reflected in the residence times of Li+ with the anions (Li), which are revealed to be much larger for [pyr14][TFSI] (up to 100 ns at the highest doping levels) than in either [EMIM][BF4] or [pyr13][FSI]. Finally, to comment on the relative kinetics of Li+ transport in each liquid, we find that while the net motion of Li+ with its solvation shell (vehicular) significantly contributes to net diffusion in all liquids, the importance of transport through anion exchange (hopping) increases at high xLi+ and in liquids with large anions.

electrolytes↗
DOE OSTI2014

Highly mobile segments in crystalline poly(ethylene oxide){sub 8}:NaPF{sub 6} electrolytes studied by solid-state NMR spectroscopy

Two types of high-crystallinity poly(ethylene oxide)/NaPF{sub 6} electrolytes with ethylene oxide (EO)/Na molar ratios of 8:1 and 6:1, termed as PEO{sub 8}:NaPF{sub 6} and PEO{sub 6}:NaPF{sub 6} with M{sub w} = 6000 g mol{sup −1} were prepared, and their ionic conductivity, structure, and segmental motions were investigated and compared. PEO{sub 8}:NaPF{sub 6} polymer electrolyte exhibits the room-temperature ionic conductivity 7.7 × 10{sup −7} S cm{sup −1} which is about five times higher than the PEO{sub 6}:NaPF{sub 6}. By variable-temperature measurements of static powder spectra and {sup 1}H spin-lattice relaxation time in rotation frame ({sup 1}H T{sub 1ρ}), we demonstrate that crystalline segments are more highly mobile in the crystalline PEO{sub 8}:NaPF{sub 6} with higher ionic conductivity than in the PEO{sub 6}:NaPF{sub 6} with lower ionic conductivity. The large-angle reorientation motion of polymer segments in the PEO{sub 8}:NaPF{sub 6} onsets at lower temperature (∼233 K) with a low activation energy 0.31 eV that is comparable with that of the pure PEO crystal. Whereas, the large-angle reorientation motion of polymer segments in the PEO{sub 6}:NaPF{sub 6} starts around 313 K with a high activation energy of 0.91 eV. As a result of the temperature-enhanced large-angle reorientations, the {sup 13}C static powder lineshape changes markedly from a low-temperature wide pattern with apparent principal values of chemical shift δ{sub 33} < δ{sub 22} < δ{sub 11} to a high-temperature narrow pattern of uniaxial chemical shift anisotropy δ{sub 33} > δ{sub 22} (δ{sub 11}). It is suggested that the segmental motion in crystalline PEO-salt complex promotes ionic conductivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Determining Proton Transport in Pseudo Catalyst Layers Using Hydrogen Pump DC and AC Techniques

Optimizing electrode morphology with a more uniform ionomer distribution is key to reducing ohmic losses and increasing electrocatalyst utilization in polymer electrolyte fuel cells (PEFCs). Inherent ionomer conductivity, volume fraction and tortuosity determine effective ionic conductivity. We use hydrogen pump (HP) method to measure effective ionic conductivity of a pseudo catalyst layer (PCL) comprised of Vulcan XC-72 carbon black and 3M 825 EW ionomer with ionomer to carbon (I/C) ratios of 0.6, 1 and 1.4 and relative humidity (RH) range of 50 to 120%. These direct current (DC) experiments are then compared with electrochemical impedance spectroscopy (EIS). Both DC and EIS methods show good agreement, indicating that EIS can be used as an alternative to DC method in HP experiment. Ionic conductivity for PCL with I/C of 1 and 1.4 was found to be about one order of magnitude higher than I/C of 0.6 for most of the RH range. At 90% RH tortuosities for I/C = 1 and 1.4 were close to 1, whereas tortuosity for I/C = 0.6 was 3. With decrease in relative humidity tortuosities increased linearly and at 50% relative humidity a PCL with I/C = 0.6 had the highest tortuosity of 6.1.

25 ENERGY STORAGE↗
DOE OSTI2023

Mixed Ionic Electronic Conducting Quaternary Perovskites: Materials by Design for Solar Thermochemical Hydrogen

The innovative research conducted by Arizona State University and Princeton University in the project "Mixed Ionic-Electronic Conducting Quaternary Perovskites: Materials by Design for Solar Thermochemical Hydrogen" marks a significant stride forward in thermochemical water splitting. Through an intricate blend of computational design and experimental validation, the project delved into the promising potential of Mixed Ionic Electronic Conducting (MIEC) perovskites. These complex materials, characterized by their unique redox-active nature and adaptability in stoichiometry, present a promising frontier for efficient solar thermochemical hydrogen production. Firstly, the research enhanced the science by utilizing state-of-the-art computational methodologies to unravel the nuanced chemical potentials of MIEC perovskites. By simulating various off-stoichiometric scenarios and redox conditions, the team was able to predict material behaviors under diverse environmental conditions, a feat unachievable through conventional experimental methodologies alone. This approach not only fast-tracks the material screening process, significantly reducing the time from laboratory re-search to practical application, but also uncovers trends and correlations that are pivotal for future materials innovation. Regarding technical effectiveness, the project stands out in its economic feasibility. Traditional methods of materials discovery are often marred by high costs and extensive timeframes, owing to the iterative nature of experimental processes. However, by employing theoretical computations and validating these findings with targeted experiments, the project introduced a cost-effective paradigm for materials discovery and the first ever prediction, synthesis, and preliminary validation of a material solely from computational and theoretical considerations. This synergy between computation and experimentation expedites the discovery of optimal materials conducive to high-efficiency solar-to-hydrogen conversion processes. Furthermore, the public stands to benefit substantially from this research. The success of MIEC perovskites in solar thermochemical applications heralds a shift towards lower cost and lower electricity input for clean hydrogen production, hence potentially impacting climate and energy resilience. By improving the efficiency of solar-to-hydrogen conversions, the research paves the way for reduced dependency on fossil fuels, addressing the urgent global need for accessible and renewable energy sources. Moreover, the project's advancements contribute to scientific literacy in renewable energy technologies, empowering society through knowledge and spurring future innovations. In essence, this research project demonstrates significant progress in the realm of advanced water splitting through solar thermochemistry. Through its groundbreaking approaches in computational materials science and its implications for real-world applications, it holds the promise of a cleaner, more energy-resilient future.

08 HYDROGEN↗
DOE OSTI2019

Tailored crosslinking of Poly(ethylene oxide) enables mechanical robustness and improved sodium-ion conductivity

We report that sodium-based energy storage systems are promising candidates for electric vehicles and grid-level energy storage applications. The advancement of sodium-based energy storage systems relies on the development of high performance sodium-ion conducting electrolytes and membranes that exhibit high ionic conductivity and mechanical stability. A crosslinked poly(ethylene oxide) based polymer electrolyte was developed that demonstrates high ionic conductivity, as well as excellent mechanical stability over a wide temperature range. Ionic conductivities up to 2.0 × 10 -4 S/cm at 20 °C and 7.1 × 10 -4 S/cm at 70 °C are achieved for the plasticized membrane, almost four orders of magnitude greater than that of the non-plasticized membrane. The membranes are mechanically robust, and the storage modulus of the membrane is maintained at ~1 MPa from -20 to 180 °C even with the addition of plasticizer. In conclusion, this study provides a synthesis approach towards the design of highly ion conducting, mechanically robust gel polymer electrolytes for Na-ion batteries, non-aqueous flow batteries, and many other applications.

25 ENERGY STORAGE↗