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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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461 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Chemical Bond Covalency in Superionic Halide Solid‐State Electrolytes

Abstract Halide solid‐state electrolytes (SSEs) are promising superionic conductors with high oxidative stability and ionic conductivity, making them attractive for all‐solid‐state lithium‐ion batteries. However, most studies have focused on ion‐stacking structures, overlooking the role of bond characteristics in ionic transport. Here, we investigate bond dynamics and the superionic transition (SIT) in bromide electrolyte, Li 3 InBr 6 , using synchrotron X‐ray techniques and ab initio molecular dynamics (AIMD) simulations. We demonstrate that the SIT in halide SSEs is driven by a thermally induced transition in bonding character (ionic to covalent) rather than a change in crystal phase. AIMD simulations further reveal enhanced Li⁺ diffusion and collective anion motion at elevated temperatures. Expanding our study to Li 3 LnBr 6 (Ln = Gd, Tb, Ho, Tm, and Lu), we confirm the widespread occurrence of SIT in this material class, with Li 3 GdBr 6 exhibiting the highest ionic conductivity (5.2 mS cm −1 at 298 K). More importantly, the ionic‐covalent transition is highly tunable through electrolyte modifications, such as cation/anion substitution and synthesis methods. Our findings provide a new perspective on ionic transport, highlighting the critical role of chemical bond characteristics in halide SSEs.

Chemistry↗
DOE OSTI2025

In‐Plane Anisotropy in van der Waals NiTeSe Ternary Alloy

Abstract The anisotropic properties of materials profoundly influence their electronic, magnetic, optical, and mechanical behaviors and are critical for a wide range of applications. In this study, the anisotropic characteristics of Ni‐based van der Waals materials, specifically NiTe 2 and its alloy NiTeSe, utilizing a combination of comprehensive scanning tunneling microscopy (STM), angle‐resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations, are explored. Unlike 1T‐NiTe 2 , which exhibits trigonal in‐plane symmetry, the substitution of Te with Se in NiTe 2 (resulting in the NiTeSe alloy) induces a pronounced in‐plane anisotropy. This anisotropy is clear in the STM topographs, which reveal a distinct linear order of charge distribution. Corroborating these observations, ARPES measurements and DFT calculations reveal an anisotropic Fermi surface centered at the point, which is notably elongated along the k y direction, leading to directional variations in in‐plane carrier velocities. Consequently, the Fermi velocity is highest along the k x direction where the linear charge distribution aligns in real space and is lowest along the k y direction. These findings offer valuable insights into the tunability of anisotropic properties in ternary transition metal dichalcogenide systems, highlighting their potential applications in the development of anisotropic electronic and optoelectronic devices.

Chemistry↗
DOE OSTI2025

Effect of Entropic Constraints on the Thermodynamics of Molecular Adsorption in Nano‐Porous Materials

Abstract Gas separation is a critical industrial process that consumes a significant amount of energy due to the widely used techniques that are currently employed. Adsorptive materials—such as metal–organic frameworks (MOFs)—show promise as an energy‐efficient alternative. Of particular current interest are novel, temperature‐dependent separation processes in MOFs, such as the recently reported separation of ternary isomeric hydrocarbon mixtures within one and the same material. However, the mechanisms of these highly desirable separations remain poorly understood. Herein, through a combination of ab initio simulations and statistical mechanics, it is shown that the temperature dependence is the result of a constraint on the guest molecule's entropic degrees of freedom when loaded into the MOF, caused by the fortuitous tight fitting of the guest inside the pore. While the framework applies to all molecular adsorption in porous media, it is essential for the description of large molecules in small pores, which is demonstrated here using the separation of C6 isomers in Ca(H 2 tcpb) as a test case. The developed framework and analysis not only reveal the reason why separation occurs but also predict the temperatures at which it takes place, thus opening the door to newly designed MOFs with tailor‐made precision.

Chemistry↗
DOE OSTI2023

Enhancing Charge Storage of Mo 2 Ti 2 C 3 MXene by Partial Oxidation

Abstract Driving the pseudocapacitive redox intercalation in 2DMXenes with neutral electrolytes is important for safer, more sustainable, and improved electrochemical charge storage. Single transition metal MXenes, such as Ti 3 C 2 , have shown great promise for energy storage, owing to their high conductivity and redox activity. Mixed metallic MXenes, such as out‐of‐plane ordered Mo 2 Ti 2 C 3 , have remained underexplored in energy storage because of the absence of redox activity in most of the electrolytes. Simultaneous structural modifications and instigating intercalation pseudocapacitance in neutral electrolytes could be a viable strategy for enhancing their electrochemical properties. Herein, a facile synthesis of partially oxidized Mo 2 Ti 2 C 3 MXene (PO‐Mo 2 Ti 2 C 3 ) exhibiting improved charge storage capability is demonstrated. Optical, structural, and spectroscopic analyses indicate the formation of oxide nanostructures upon thermal oxidation of Mo 2 Ti 2 C 3 . This leads to an enhanced energy storage capability with remarkably improved cyclability as well as a high Coulombic efficiency in a neutral LiCl electrolyte. This work highlights the importance of structural modifications of MXenes to enhance their charge storage and shows the promise of less explored double transition metal MXenes in energy storage.

Chemistry↗
DOE OSTI2026

A Permanently Porous Chalcogen-Bonded Organic Framework

The nature of connectivity between constituent atomic or molecular building blocks is fundamental in shaping the properties and functionality of materials. The extrapolation of emergent interatomic interactions to enable functional materials has driven transformative technological advancements. However, the bonding interactions used in material design have been largely static since the emergence of dynamic covalent chemistry ~30 years ago. Here we demonstrate that non-covalent chalcogen bonding (Ch-bonding) is a distinct mode of interatomic connectivity for constructing functional materials by design. This is established by leveraging self-complementary assembly of 1,2,5-telluradiazole moieties to construct a honeycomb-type permanently porous Ch-bonded organic framework, assembled and stabilized solely through non-covalent Te...N contacts. Empirical and computational studies of electronic structure, structural healing and lattice dynamics highlight the pi-type electronic communication, controlled assembly and modulated lattice dynamics in Trip3Tez-I arising directly from the unique nature of the Te...N Ch-bonding that holds substantial implications for next generation crystalline semiconductors. In addition to introducing a distinct class of permanently porous frameworks, this work establishes Ch-bonding as a programmable molecular tool for constructing functional materials with distinct properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Smart Droplets Stabilized by Designer Surfactants: From Biomimicry to Active Motion to Materials Healing

The science and technologies of emulsion droplets have been a long‐term focus of extensive research endeavors for their practical utility across a breadth of industries, including pharmaceutical products, oil recovery processes, and the food sciences. However, with advances in materials chemistry and characterization tools, new emerging areas are arising with a focus on “smart droplets”. The versatility of emulsion droplets across is based on their ability to partition and create isolated systems with properties defined by the liquid–liquid interface, while preparative routes allow manipulation of droplet size, stability, and encapsulated contents. As described in this article, significant efforts are being devoted to creating new types of droplets by “activating” this interface through the incorporation of reactive structures that trigger droplet response to applied or environmental stimuli (e.g., pH, temperature, salt, or external fields). Moreover, parallels between droplets and live cells inspire efforts to conceive systems that resemble biological motifs or that can produce cellular behaviors that imitate biology (e.g., swarming, communication, or motion). Here, the authors highlight recent advances in smart droplets, with emphasis on organic, polymer, and/or particle surfactants that give rise to inter‐droplet communication (via aggregation, fusion, division, or mass transfer), droplet vehicles for controlled delivery, autonomous droplet motion, and tunable emulsion inversion. Especially emphasized is the macromolecular design to produce reactive and functional surfactants, which are crucial to responsive droplet behavior and their underlying mechanisms. More generally, the exquisite interplay between materials science and biology inspires the review of this research area that provides unique opportunities for insight and inspiration into the capabilities of new droplet designs.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Should I stay or should I flow? An exploration of phase‐separated metallosupramolecular liquid crystal polymers

Abstract Dynamic liquid crystalline polymers (dLCPs) incorporate both liquid crystalline mesogens and dynamic bonds into a single polymeric material. These dual functionalities impart order‐dependent thermo‐responsive mechano‐optical properties and enhanced reprocessability/programmability enabling their use as soft actuators, adaptive adhesives, and damping materials. While many previous works studying dynamic LCPs utilize dynamic covalent bonds, metallosupramolecular bonds provide a modular platform where a series of materials can be accessed from a single polymeric feedstock through the variation of the metal ion used. A series of dLCPs were prepared by the addition of metal salts to a telechelic 2,6‐bisbenzimidazolylpyridine (Bip) ligand endcapped LCP to form metallosupramolecular liquid crystal polymers (MSLCPs). The resulting MSLCPs were found to phase separate into hard and soft phases which aids in their mechanical robustness. Variations of the metal salts used to access these materials allowed for control of the thermomechanical, viscoelastic, and adhesive properties with relaxations that can be tailored independently of the mesogenic transition. This work demonstrates that by accessing phase separation through the incorporation of metallosupramolecular moieties, highly processable yet robust MSLCP materials can be realized. This class of materials opens the door to LCPs with bulk flow behavior that can also be utilized as multi‐level adhesives.

Chemistry↗
DOE OSTI2025

Effect of Preparation Conditions of Fe@SiO2 Catalyst on Its Structure Using High-Pressure Activity Studies in a 3D-Printed SS Microreactor

Fischer–Tropsch synthesis (FTS) in a 3D-printed stainless steel (SS) microchannel microreactor was investigated using Fe@SiO2 catalysts. The catalysts were prepared by two different techniques: one pot (OP) and autoclave (AC). The mesoporous structure of the two catalysts, Fe@SiO2 (OP) and Fe@SiO2 (AC), ensured a large contact area between the reactants and the catalyst. They were characterized by N2 physisorption, H2 temperature-programmed reduction (H2-TPR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron microscopy (XPS), and thermogravimetric analysis–differential scanning calorimetry (TGA-DSC) techniques. The AC catalyst had a clear core–shell structure and showed a much greater surface area than that prepared by the OP method. The activities of the catalysts in terms of FTS were studied in the 200–350 °C temperature range at 20-bar pressure with a H2/CO molar ratio of 2:1. The Fe@SiO2 (AC) catalyst showed higher selectivity and higher CO conversion to olefins than Fe@SiO2 (OP). Stability studies of both catalysts were carried out for 30 h at 320 °C at 20 bar with a feed gas molar ratio of 2:1. The Fe@SiO2 (AC) catalyst showed higher stability and yielded consistent CO conversion compared to the Fe@SiO2 (OP) catalyst.

Biochemistry & Molecular Biology↗
DOE OSTI2024

High-Density Capacitive Energy Storage in Low-Dielectric-Constant Polymer PMMA/2D Mica Nanofillers Heterostructure Composite

The ubiquitous, rising demand for energy storage devices with ultra-high storage capacity and efficiency has drawn tremendous research interest in developing energy storage devices. Dielectric polymers are one of the most suitable materials used to fabricate electrostatic capacitive energy storage devices with thin-film geometry with high power density. In this work, we studied the dielectric properties, electric polarization, and energy density of PMMA/2D Mica nanocomposite capacitors where stratified 2D nanofillers are interfaced between the multiple layers of PMMA thin films using two heterostructure designs of the capacitors, PMMA/2D Mica/PMMA (PMP) and PMMA/2D Mica/PMMA/2D Mica/PMMA (PMPMP). The incorporation of a 2D Mica nanofiller in the low-dielectric-constant PMMA leads to an enhancement in the dielectric constant, with ∆ε ~ 15% and 53% for PMP and PMPMP heterostructures at room temperature. Additionally, a significant improvement in discharged energy density was measured for the PMPMP capacitor (Ud ~ 38 J/cm3 at 825 MV/m) compared to the pristine PMMA (Ud ~ 9.5 J/cm3 at 522 MV/m) and PMP capacitors (Ud ~ 19 J/cm3 at 740 MV/m). This excellent capacitive and energy storage performance of the PMMA/2D Mica heterostructure nanocomposite may inform the fabrication of thin-film, high-density energy storage capacitor devices for potential applications in various platforms.

Biochemistry & Molecular Biology↗
DOE OSTI2024

Resonant Metasurfaces with Van Der Waals Hyperbolic Nanoantennas and Extreme Light Confinement

This work reports on a metasurface based on optical nanoantennas made of van der Waals material hexagonal boron nitride. The optical nanoantenna made of hyperbolic material was shown to support strong localized resonant modes stemming from the propagating high-k waves in the hyperbolic material. An analytical approach was used to determine the mode profile and type of cuboid nanoantenna resonances. An electric quadrupolar mode was demonstrated to be associated with a resonant magnetic response of the nanoantenna, which resembles the induction of resonant magnetic modes in high-refractive-index nanoantennas. The analytical model accurately predicts the modes of cuboid nanoantennas due to the strong boundary reflections of the high-k waves, a capability that does not extend to plasmonic or high-refractive-index nanoantennas, where the imperfect reflection and leakage of the mode from the cavity complicate the analysis. In the reported metasurface, excitations of the multipolar resonant modes are accompanied by directional scattering and a decrease in the metasurface reflectance to zero, which is manifested as the resonant Kerker effect. Van der Waals nanoantennas are envisioned to support localized resonances and can become an important functional element of metasurfaces and transdimensional photonic components. By designing efficient subwavelength scatterers with high-quality-factor resonances, this work demonstrates that this type of nanoantenna made of naturally occurring hyperbolic material is a viable substitute for plasmonic and all-dielectric nanoantennas in developing ultra-compact photonic components.

Chemistry↗
DOE OSTI2024

Mechanically and Thermally Robust Gel Electrolytes Built from A Charged Double Helical Polymer

Polymer electrolytes have received tremendous interest in the development of solid-state batteries, but often fall short in one or more key properties required for practical applications. Herein, a rigid gel polymer electrolyte prepared by immobilizing a liquid mixture of a lithium salt and poly(ethylene glycol) dimethyl ether with only 8 wt% poly(2,2′-disulfonyl-4,4′-benzidine terephthalamide) (PBDT) is reported. The high charge density and rigid double helical structure of PBDT lead to formation of a nanofibrillar structure that endows this electrolyte with stronger mechanical properties, wider temperature window, and higher battery rate capability compared to all other poly(ethylene oxide) (PEO)-based electrolytes. The ion transport mechanism in this rigid polymer electrolyte is systematically studied using multiple complementary techniques. Li/LiFePO 4 cells show excellent capacity retention over long-term cycling, with thermal cycling reversibility between ambient temperature and elevated temperatures, demonstrating compelling potential for solid-state batteries targeting fast charging at high temperatures and slower discharging at ambient temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Technoeconomic and Emissions Analysis of the Hybrid Redox Process for the Production of Acetic Acid with CO 2 Utilization

The production of oxygenated hydrocarbons, such as acetic acid, using captured CO 2 is a promising pathway to reduce greenhouse gas emissions in the chemical industry. The use of a chemical looping‐based hybrid redox process (HRP) is proposed to convert CO 2 and natural gas into separate CO and syngas streams that can be used to produce various commodity oxygenates, while allowing the beneficial utilization of captured CO 2 . Here, a detailed technoeconomic analysis of HRP applied to the production of acetic acid is presented. Emissions and energy analyses show the ability of HRP to lower the CO 2 emissions for acetic acid synthesis by 74% compared to a conventional steam and autothermal reforming route. HRP also offers a potential 34% reduction in capital costs. Compared to a dry reforming based acetic acid production route, HRP has the potential for significantly lower costs. If integrated with a low carbon energy source, HRP has the potential to achieve a negative emission of greenhouse gas (‐0.50 kg CO 2 per kg acetic acid).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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 OSTI2026

Role of Amorphous Chains in Nanoplastic Formation from Semicrystalline Polymers

Semicrystalline polymers, e.g., polyethylene terephthalate (PET), release micro- (100 nm to 1 mm) and nanoplastics (up to 100 nm) [MNPL] when they are degraded under quiescent conditions. However, the exact molecular mechanisms leading to material fragmentation into MNPL are unknown. Here, we monitor the evolution of chain molecular weight and the MNPL production kinetics during hydrolysis of PET pellets. We find that only ~0.6% of the amorphous phase ester bonds are hydrolyzed at the onset of MNPL release. Then, by combining a random scission model with measured amorphous spacings, we estimate that only ~15% of the stress transmitters in the amorphous phase, namely, bridges and entangled loops, have failed by this point. Thus, spontaneous fragmentation of the semicrystalline nanostructure occurs despite significant intercrystalline connectivity. We resolve this apparent contradiction by proposing that fragmentation can only occur when progressive tie-chain scission causes the material to undergo the ductile/brittle transition. Mechanistically, we speculate that the internal stresses responsible for material fragmentation are caused by processing (i.e., residual stresses) and/or sample densification induced by chemi-crystallization. We discuss additional factors that may affect our analysis and thus require further investigation, such as skin-core effects, preferential degradation of stress transmitters and/or recrystallization processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Observation of Extraordinary Vibration Scatterings Induced by Strong Anharmonicity in Lead‐Free Halide Double Perovskites

Abstract Lead‐free halide double perovskites provide a promising solution for the long‐standing issues of lead‐containing halide perovskites, i.e., the toxicity of Pb and the low stability under ambient conditions and high‐intensity illumination. Their light‐to‐electricity or thermal‐to‐electricity conversion is strongly determined by the dynamics of the corresponding lattice vibrations. Here, the measurement of lattice dynamics is presented in a prototypical lead‐free halide double perovskite(Cs 2 NaInCl 6 ). The quantitative measurements and first‐principles calculations show that the scatterings among lattice vibrations at room temperature are at the timescale of ≈1 ps, which stems from the extraordinarily strong anharmonicity in Cs 2 NaInCl 6 . Further the degree of anharmonicity of each type of atom is quantitatively characterized in the Cs 2 NaInCl 6 single crystal, which stems from the interatomic forces, and demonstrate that this strong anharmonicity is synergistically contributed by the bond hierarchy, the tilting of the NaCl 6 and InCl 6 octahedral units, and the rattling of Cs + ions. Consequently, the crystalline Cs 2 NaInCl 6 possesses an ultralow thermal conductivity of ≈0.43 W mK −1 at room temperature, and a weak temperature dependence ofT −0.41 . These findings uncovered the underlying mechanisms behind the dynamics of lattice vibrations in double perovskites, which can largely benefit the design of optoelectronics and thermoelectrics based on halide double perovskites.

Chemistry↗
DOE OSTI2025

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↗
DOE OSTI2025

Cyclic Peptides for Lanthanide Binding

Lanthanide ions are difficult to separate from one another due to their similar chemical properties. The discovery of lanthanide-binding peptides and proteins in nature has led to an increased interest in the possibility of utilizing the strong binding of peptides to lanthanide ions for their separations; as such, there has been an effort to identify or design peptides with improved lanthanide binding and selectivity toward particular lanthanide ions. Here, in this study, we designed and characterized lanthanide-binding cyclic peptides (LBCPs) with molecular dynamics simulations, electronic structure calculations, and emission spectroscopy. Luminescent decay measurements were done to determine the number of water molecules coordinated to the Eu 3+ ion in Eu-LBCP complexes and compare to the predicted number of water molecules by computation to assess the lanthanide-binding affinity of LBCPs. Measured stability constants show binding of the LBCPs to the Eu 3+ ion with stronger than micromolar affinity. We were able to identify multiple peptides that selectively bind to middle lanthanides. We describe the structural basis of the lanthanide-binding selectivity trend with strongest binding to the middle lanthanides, followed by the heavier lanthanides, and finally to the lighter ions.

ions↗
DOE OSTI2024

Mitigating Sodium Ordering for Enhanced Solid Solution Behavior in Layered NaNiO 2 Cathodes

The O-type layered nickel oxides suffer from undesired cooperative Jahn–Teller distortion stemming from Ni 3+ ions and undergo multiple biphasic structural transformations during the insertion/extraction of large Na + ions, posing a significant challenge to stabilize the structural integrity. We present here a systematic investigation of the impact of substituting 5 % divalent (Mg 2+ ) or trivalent (Al 3+ or Co 3+ ) ions for Ni 3+ to alleviate Na + ion ordering and perturb the Jahn–Teller effect to enhance structural stability. Here, we gauge a fundamental understanding of the Mg−O and Na−O or Mg−O−Na bonding interactions, noting that the ionicity of the Mg−O bond deshields the electronic cloud of oxygen from Na + ions. Furthermore, calculations of the Van Vleck distortion modes reveal a relaxation of NiO 6 octahedra from Jahn–Teller distortion and a reduced electron density at the interlayer with Mg 2+ substitution. Long-range (operando X-ray diffraction) and short-range (magic angle spinning nuclear magnetic resonance) structural analyses provide insights into reduced ordering, allowing a stable continuous solid solution. Overall, Mg-substitution results in a high-capacity retention of ~96 % even after 100 cycles, showcasing the potential of this strategy for overcoming the structural instabilities and enhancing the performance of sodium-ion batteries.

25 ENERGY STORAGE↗