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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Amorphous ZrCl 4 -Based Superionic Conductor as a Cost-Effective Solid Electrolyte for Batteries

Developing highly conductive and cost-effective solid electrolytes is essential for the commercialization of all-solid-state batteries (ASSBs). Zr-based halide electrolytes hold great promise due to their low estimated cost and high oxidation stability. However, the ionic conductivities of most of them are not high enough to enable moderate- and high-rate cycling of ASSBs. Here, fast ion transport is achieved in a group of cost-effective ZrCl 4 -based electrolytes via a design strategy to create highly disordered amorphous structures. Amorphous Li 0.8 ZrCl 4 (SO 4 ) 0.4 , with a low estimated cost of $21 kg –1 , achieves an ionic conductivity of 1.86 mS cm –1 at 25 °C. It also shows a high oxidation limit of 4.5 V vs Li/Li + and good compatibility with high-voltage cathodes, as demonstrated by the stable cycling of ASSBs (73.7% capacity retention after 1000 cycles at 1 C). Synchrotron X-ray diffraction, pair distribution function analysis, and electrochemical impedance spectroscopy reveal that the outstanding conductivity of these amorphous electrolytes is closely related to their short-range and medium-range ordering, revealing new insights for designing high-performance, cost-effective solid electrolytes.

Zhang, Guangxing [Georgia Institute of Technology,↗
DOE OSTI2024

Integrated photonic encoder for low power and high-speed image processing

Abstract Modern lens designs are capable of resolving greater than 10 gigapixels, while advances in camera frame-rate and hyperspectral imaging have made data acquisition rates of Terapixel/second a real possibility. The main bottlenecks preventing such high data-rate systems are power consumption and data storage. In this work, we show that analog photonic encoders could address this challenge, enabling high-speed image compression using orders-of-magnitude lower power than digital electronics. Our approach relies on a silicon-photonics front-end to compress raw image data, foregoing energy-intensive image conditioning and reducing data storage requirements. The compression scheme uses a passive disordered photonic structure to perform kernel-type random projections of the raw image data with minimal power consumption and low latency. A back-end neural network can then reconstruct the original images with structural similarity exceeding 90%. This scheme has the potential to process data streams exceeding Terapixel/second using less than 100 fJ/pixel, providing a path to ultra-high-resolution data and image acquisition systems.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons

Understanding the origin of electron–phonon coupling in lead halide perovskites is key to interpreting and leveraging their optical and electronic properties. Here we show that photoexcitation drives a reduction of the lead–halide–lead bond angles, a result of deformation potential coupling to low-energy optical phonons. We accomplish this by performing femtosecond-resolved, optical-pump–electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in nanocrystals of FAPbBr 3 . Our results indicate a stronger coupling in FAPbBr 3 than CsPbBr 3 . We attribute the enhanced coupling in FAPbBr 3 to its disordered crystal structure, which persists down to cryogenic temperatures. We find the reorganizations induced by each exciton in a multi-excitonic state constructively interfere, giving rise to a coupling strength that scales quadratically with the exciton number. This superlinear scaling induces phonon-mediated attractive interactions between excitations in lead halide perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Active Learning-driven Quantitative Synthesis-Structure-Property Relations for Improving Performance and Revealing Active Sites of Nitrogen-Doped Carbon for the Hydrogen Evolution Reaction

While quantitative structure-properties relations (QSPRs) have been developed successfully in multiple fields, catalyst synthesis affects structure and in turn performance, making simple QSPRs inadequate. Furthermore, catalysts often have multiple active sites preventing one from obtaining insights into structure-property relations. Here, we develop a data-driven quantitative synthesis-structure-property relation (QS2PRs) methodology to elucidate correlations between catalyst synthesis conditions, structural properties as well as observed performance and to provide fundamental insights into active sites and a systematic way to optimize practical catalysts. Here, we demonstrate the approach to the synthesis of nitrogen-doped catalysts (NDC) made via pyrolysis for the performance of the electrochemical hydrogen evolution reaction (HER), quantified by the onset potential and the current density. We determine crystallinity, nitrogen species type and fraction, surface area, and pore structure of the NDC’s using XRD, XPS, and BET characterization. We demonstrated that an active learning-based optimization combined with various elementary machine learning tools (regression, principal component analysis, partial least squares) can efficiently identify optimum pyrolysis conditions to tune structural characteristics and performance with concomitant savings in materials and experimental time. Unlike previous reports on the importance of pyridinic or graphitic nitrogen, we discover that the electrochemical performance is not driven by a single catalyst property; rather, it arises from a multivariate influence of nitrogen dopants, pore structure and disorder in the NDC materials. Identification of active sites can help mechanistic understanding and further catalyst improvement.

42 ENGINEERING↗
DOE OSTI2025

A polysulfide/ferricyanide redox flow battery with extended cycling

The inexpensive sulfur raw material is promising to enable cost-effective redox flow batteries for long duration energy storage. But the catastrophic through-membrane crossover of polysulfides remains a severe challenge resulting in irreversible performance degradation and short cycle life. In this work, we demonstrate that use of a permselective cation exchange membrane yields a two orders of magnitude enhancement in polysulfide retention compared to the benchmark Nafion membrane. Combined physico-chemical, spectroscopic, and microscopic analyses suggest more disordered sidechain structures, which lead to the more hydrophobic nature and smaller hydrophilic domains in the membrane. The microstructural features contribute to the effective mitigation of polysulfide crossover. As a result, the cycle life of polysulfide/ferricyanide flow cells is boosted over a substantially extended test time. This finding sheds light on the fundamental membrane factors that cause polysulfide permeation and can provide feasible directions in the development of permselective membranes for polysulfide flow batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Structural, electronic, and magnetic properties of CoFeVGe-based compounds: Experiment and theory

We have carried out a combined theoretical and experimental investigation of both stoichiometric and nonstoichiometric CoFeVGe alloys. In particular, we have investigated CoFeVGe, Co 1.25 Fe 0.75 VGe, Co 0.75 Fe 1.25 VGe, and CoFe 0.75 VGe bulk alloys. Our first principles calculations suggest that all four alloys show ferromagnetic order, where CoFeVGe, Co 1.25 Fe 0.75 VGe, and Co 0.75 Fe 1.25 VGe are highly spin polarized with spin polarization values of over 80%. However, the spin polarization value of CoFe 0.75 VGe is only about 60%. We have synthesized all four samples using arc melting and high-vacuum annealing at 600 °C for 48 hours. The room temperature x-ray diffraction of these samples exhibits a cubic crystal structure with disorder. All the samples show single magnetic transitions at their Curie temperatures, where the Curie temperature and high field (3T) magnetization are 288 K and 42 emu/g; 305 K and 1.5 emu/g; 238 K and 39 emu/g; and 306 K and 35 emu/g for CoFeVGe, Co 1.25 Fe 0.75 VGe, Co 0.75 Fe 1.25 VGe, and CoFe 0.75 VGe, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Bulk and element-specific magnetism of medium-entropy and high-entropy Cantor-Wu alloys

Magnetic Compton scattering, x-ray magnetic circular dichroism spectroscopy, and bulk magnetometry measurements are performed on a set of medium- (NiFeCo and NiFeCoCr) and high-entropy (NiFeCoCrPd and NiFeCoCrMn) Cantor-Wu alloys. The bulk spin momentum densities determined by magnetic Compton scattering are remarkably isotropic, and this is a consequence of the smearing of the electronic structure by disorder scattering of the electron quasiparticles. Nonzero x-ray magnetic circular dichroism signals are observed for every element in every alloy indicating differences in the populations of the majority and minority spin states implying finite magnetic moments. When Cr is included in the solid solution, the Cr spin moment is unambiguously antiparallel to the total magnetic moment, while a vanishingly small magnetic moment is observed for Mn, despite calculations indicating a large moment. Some significant discrepancies are observed between the experimental bulk and surface magnetic moments. Furthermore, despite the lack of quantitative agreement, the element-specific surface magnetic moments seem to be qualitatively reasonable.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Lithium-compatible and air-stable vacancy-rich Li 9 N 2 Cl 3 for high–areal capacity, long-cycling all–solid-state lithium metal batteries

Attaining substantial areal capacity (>3 mAh/cm 2 ) and extended cycle longevity in all–solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich Li 9 N 2 Cl 3 SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high–areal capacity, long-lasting all–solid-state lithium metal batteries. The Li 9 N 2 Cl 3 facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm 2 and 10 mAh/cm 2 due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 cathode-based all–solid-state batteries, we achieve substantial cycling stability (90.35% capacity retention over 1500 cycles at 0.5 C) and high areal capacity (4.8 mAh/cm 2 in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands.

25 ENERGY STORAGE↗
DOE OSTI2024

Zero-Power Analog Optical Processing

The motivation behind this research is the growing challenge of handling the massive amounts of data generated by modern imaging systems. Conventional digital image processing techniques are struggling to keep pace with the demands of high-resolution and high-speed imaging systems for remote sensing due to their high-power consumption and data storage requirements. We present a novel approach based on analog photonics to address this challenge. The proposed system utilizes a silicon-photonics-based image encoder positioned after image formation and initial optical-to-electrical conversion. The photonic encoder compresses image data using a passive disordered photonic structure to perform kernel-type random projections of the raw data. The compressed data is then processed by a back-end neural network, which reconstructs the original image with high fidelity (structural similarity exceeding 90%). Our proposed approach has the potential to compress images with ~ 1000X lower power consumption compared to digital approaches with data rates exceeding 1 terapixel/second.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Metal-Catalyzed Thermo-Catalytic Decomposition and Continuous Catalyst Generation

In this study, metal dusting is utilized to initiate a two-stage thermo-catalytic decomposition (TCD) process. Stage 1 starts with metal-catalyzed TCD, and in stage 2 the metal-catalyzed carbon catalyzes additional TCD. TEM is presented of the early- versus late-stage TCD to qualitatively illustrate the second-stage TCD by the metal-catalyzed carbons. Corresponding SEM illustrates differences in growth type and surface density between early versus late reaction times, with backscattered imaging differentiating the first- versus second-stage TCD. TGA supports the microscopic inference of a second carbon phase by the presence of an early (low-temperature) reaction peak, characteristic of low-structure or disordered carbon as the second-stage TCD carbon. Raman analysis confirms that the second-stage carbon deposit is more disordered and unstructured, especially at 1000 °C, supported by the ID/IG and La value changes from 0.068 to 0.936 and 65 nm to 4.7 nm, respectively. To further confirm second-stage TCD occurrence upon pre-catalyzed carbons, two carbon blacks are tested. Exposing a combination of edge and basal or exclusively basal sites for the graphitized form, they afford a direct comparison of TCD carbon nanostructure dependence upon the initial carbon catalyst nanostructure. Pre-oxidation of the stainless-steel wool (SSW) prior to TCD is advantageous, accelerating TCD rates and increasing carbon yield relative to the nascent SSW for an equivalent reaction duration.

Chemistry↗
DOE OSTI2023

Anisotropic Properties of Epitaxial Ferroelectric Lead-Free 0.5[Ba(Ti 0.8 Zr 0.2 )O 3 ]-0.5(Ba 0.7 Ca 0.3 )TiO 3 Films

As the energy demand is expected to double over the next 30 years, there has been a major initiative towards advancing the technology of both energy harvesting and storage for renewable energy. In this work, we explore a subset class of dielectrics for energy storage since ferroelectrics offer a unique combination of characteristics needed for energy storage devices. We investigate ferroelectric lead-free 0.5[Ba(Ti 0.8 Zr 0.2 )O 3 ]-0.5(Ba 0.7 Ca 0.3 )TiO 3 epitaxial thin films with different crystallographic orientations grown by pulsed laser deposition. We focus our attention on the influence of the crystallographic orientation on the microstructure, ferroelectric, and dielectric properties. Our results indicate an enhancement of the polarization and strong anisotropy in the dielectric response for the (001)-oriented film. The enhanced ferroelectric, energy storage, and dielectric properties of the (001)-oriented film is explained by the coexistence of orthorhombic-tetragonal phase, where the disordered local structure is in its free energy minimum.

36 MATERIALS SCIENCE↗
NASA NTRS1972

Fracture Behavior in Nylon 6 Fibers

Electron paramagnetic resonance (EPR) techniques are used to determine the number of free radicals produced during deformation leading to fracture of nylon 6 fibers. A reaction rate molecular model is proposed to explain some of the deformation and bond rupture behavior leading to fracture. High-strength polymer fibers are assumed to consist of a sandwich structure of disordered and ordered regions along the fiber axis. In the disordered or critical flaw regions, tie chains connecting the ordered or crystalline block regions are assumed to have a statistical distribution in length. These chains are, therefore, subjected to different stresses. The effective length distribution was determined by EPR. The probability of bond rupture was assumed to be controlled by reaction-rate theory with a stress-aided activation energy and behavior of various loadings determined by numerical techniques. The model is successfully correlated with experimental stress, strain, and bond rupture results for creep, constant rate loadings, cyclic stress, stress relaxation and step strain tests at room temperature.

Lloyd, B. A.↗
NASA NTRS1999

Effective Forces Between Colloidal Particles

Colloidal suspensions have proven to be excellent model systems for the study of condensed matter and its phase behavior. Many of the properties of colloidal suspensions can be investigated with a systematic variation of the characteristics of the systems and, in addition, the energy, length and time scales associated with them allow for experimental probing of otherwise inaccessible regimes. The latter property also makes colloidal systems vulnerable to external influences such as gravity. Experiments performed in micro-ravity by Chaikin and Russell have been invaluable in extracting the true behavior of the systems without an external field. Weitz and Pusey intend to use mixtures of colloidal particles with additives such as polymers to induce aggregation and form weak, tenuous, highly disordered fractal structures that would be stable in the absence of gravitational forces. When dispersed in a polarizable medium, colloidal particles can ionize, emitting counterions into the solution. The standard interaction potential in these charged colloidal suspensions was first obtained by Derjaguin, Landau, Verwey and Overbeek. The DLVO potential is obtained in the mean-field linearized Poisson-Boltzmann approximation and thus has limited applicability. For more precise calculations, we have used ab initio density functional theory. In our model, colloidal particles are charged hard spheres, the counterions are described by a continuum density field and the solvent is treated as a homogeneous medium with a specified dielectric constant. We calculate the effective forces between charged colloidal particles by integrating over the solvent and counterion degrees of freedom, taking into account the direct interactions between the particles as well as particle-counterion, counterion-counterion Coulomb, counterion entropic and correlation contributions. We obtain the effective interaction potential between charged colloidal particles in different configurations. We evaluate two- and three-body forces in the bulk as well as study the influence of soft walls. We qualitatively explain the effects of the walls on the forces and demonstrate that many-body effects are negligible in our system. With adjustments in the parameters, the DLVO pair-potential can describe the results quantitatively. Besides electrostatic interactions, entropic depletion effects that arise from (hard-core) exclusion play an important role in determining the behavior of multi-component colloidal suspensions. A standard theory for depletion forces is due to Asakura and Oosawa and is based on the ideal gas approximation. To go beyond this approximation, we have studied entropic forces in molecular dynamics simulations of systems of hard spheres (the effects of the solvent have been ignored). The effective depletion forces for these systems can be found either from equilibrium distribution functions or from direct momentum transfer calculations. Our results obtained by either method show qualitative differences from the Asakura-Oosawa forces, indicating a longer range, higher value at contact and most importantly a more complicated structure, comprising of several maxima and minima. Our calculations include the determination of effective forces between two spheres, a hard sphere and a wall, and the behavior of a hard sphere near a step-edge and a corner. We also demonstrate that such entropic forces do not necessarily satisfy pairwise additivity.

Tehver, Riina↗
NASA NTRS2005

Pyrolytic Synthesis of Carbon Nanotubes from Sucrose on a Mesoporous Silicate

Multiwall carbon nanotubes were synthesized from sucrose by a pyrolytic technique using mesoporous MCM-41 silicate templates without transition metal catalysts. The Nanotubes were examined in the carbon/silicate composite and after dissolution of the silicate. High resolution transmission electron microscopy study of the multiwall nanotubes showed them to be 15 nm in diameter, 200 nm in length and close-ended. There was variation in crystallinity with some nanotubes showing disordered wall structures.

Abdel-Fattah, Tarek↗
DOE OSTI2020

Dynamic clay microstructures emerge via ion complexation waves

Clays control carbon, water and nutrient transport in the lithosphere, promote cloud formation5 and lubricate fault slip through interactions among hydrated mineral interfaces. Clay mineral properties are difficult to model because their structures are disordered, curved and dynamic. Consequently, interactions at the clay mineral-aqueous interface have been approximated using electric double layer models based on single crystals of mica and atomistic simulations. We discover that waves of complexation dipoles at dynamically curving interfaces create an emergent long-range force that drives exfoliation and restacking over time- and length-scales that are not captured in existing models. Curvature delocalizes electrostatic interactions in ways that fundamentally differ from planar surfaces, altering the ratio of ions bound to the convex and concave sides of a layer. Multiple-scattering reconstruction of low-dose energy-filtered cryo electron tomography enabled direct imaging of ion complexes and electrolyte distributions at hydrated and curved mineral interfaces with {\aa}ngstrom resolution over micron length scales. Layers exfoliate and restack abruptly and repeatedly over timescales that depend strongly on the counterion identity, demonstrating that the strong coupling between elastic, electrostatic and hydration forces in clays promote collective reorganization previously thought to be a feature only of active matter.

Whittaker, Michael L↗
DOE OSTI2024

Fluorinated cation-disordered rocksalt materials and methods of making thereof

This disclosure provides systems, methods, and apparatus related to lithium metal oxyfluorides. In one aspect, a method for manufacturing a lithium metal oxyfluoride having a general formula Li 1+x (MM′) z O 2-y F y , with 0.6 ≤ z ≤ 0.95, 0 < y ≤ 0.67, and 0.0 5 ≤ x ≤ 0.4, the lithium metal oxyfluoride having a cation-disordered rocksalt structure, includes: providing at least one lithium-based precursor; providing at least one redox-active transition metal-based precursor; providing at least one redox-inactive transition metal-based precursor; providing at least one fluorine-based precursor comprising a fluoropolymer; and mixing the at least one lithium-based precursor, the at least one redox-active transition metal-based precursor, the at least redox-inactive transition metal-based precursor, and the at least one fluorine-based precursor comprising a fluoropolymer to form a mixture.

Ahn, Juhyeon↗
DOE OSTI2021

High temperature transition aluminas in gamma-Al2O3: Review

High temperature treated transition aluminas display adsorptive and catalytic properties that are in many ways comparable to those of their low temperature counterpart gamma-Al2O3. While being important industrial catalysts as well as catalytic supports, their very basic crystallographic and structural characteristics remain poorly understood and thus actively studied. In this review, we critically examine the crystallography and structural complexity of these materials. Specifically, we address the crystallography of delta- and theta-Al2O3 polymorphs and show how structural intergrowth and disorder are accommodated in these phases. The structural complexity at the scale of overall microstructure is also examined, and the challenges and recent progress in quantification of the structure at ensemble level are discussed. Most pertinently to catalysis, we review the surfaces properties of high temperature treated Al2O3 and discuss the implications for understanding attributes relevant to heterogeneous catalysis.

Kovarik, Libor↗