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At least 1,531 records · Page 85

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DOE OSTI2025

Substituent size versus metal binding of inhibitors with variants of influenza endonuclease

The influenza virus causes a significant burden of illness each year. Although vaccination is the most effective method to prevent seasonal influenza infection, viral escape mechanisms make vaccine composition difficult to predict. Antivirals are crucial for decreasing rates of morbidity and mortality from influenza viral infection. The newest anti-influenza drugs target the RNA-dependent RNA polymerase acidic N-terminal (PA N ) endonuclease, a critical component of influenza viral replication machinery. This study examines the structure of inhibitors of PAN that utilize a hydroxypyridinone-based metal-binding pharmacophore (MBP). Specifically, this report explores how the size of substituent groups impacts the binding conformation and affinity of a series of compounds against both wild-type (WT) and resistance mutant strains, I38T and E23K. Co-crystal structures revealed that the distance between compounds and enzyme residue 38 was conserved to maintain strong interactions, resulting in deviations from ideal coordination geometries at the active site metal centers. This suggests the interactions with residue 38 with each compound is important and can impact inhibitor potency as a consequence of distortions in the metal binding geometry of the compounds.

Endonuclease↗

DOE OSTI2025

Measuring Solvation Interactions of Deep Eutectic Solvents Formed by Metal Chlorides and an Imidazolium Salt by Inverse Gas Chromatography

Deep eutectic solvents (DESs) represent a class of solvents that offer a number of advantages including minimal toxicity, affordability, low vapor pressure, and simple, environmentally friendly preparation methods. They have found utility in areas, such as gas absorption, metal plating, and extractions. However, the relationship between their solvation properties and chemical composition remains poorly understood. In this study, a broad range of Type I DESs composed of metal chlorides and an imidazolium salt were prepared, employed as gas chromatographic stationary phases, and characterized using the Abraham solvation parameter model by inverse gas chromatography. The Abraham solvation parameter model allows for the study of DES solvation properties and the effects of varying structural components on system constants using a linear-free energy relationship. The DESs were investigated by systematically varying their composition, including the type of metal chloride and the molar ratio between the metal chloride and the imidazolium salt. The results show that hydrogen bond acidity, hydrogen bond basicity, and dipolarity/polarizability interactions are strongly influenced by the type of metal chloride within the DES and the ratio of metal chloride to imidazolium salt in the eutectic mixture. Furthermore, a column pretreatment procedure is presented that enables the effective coating of highly polar DESs onto open tubular capillary gas chromatography columns.

deep eutectic solvent↗

NASA NTRS2016

Evolution of Shock Melt Compositions in Lunar Regoliths

Space weathering processes - driven primarily by solar wind ion and micrometeorite bombardment, are constantly changing the surface regoliths of airless bodies, such as the Moon. It is essential to study lunar soils in order to fully under-stand the processes of space weathering, and how they alter the optical reflectance spectral properties of the lunar surface relative to bedrock. Lunar agglutinates are aggregates of regolith grains fused together in a glassy matrix of shock melt produced during micrometeorite impacts into the lunar regolith. The formation of the shock melt component in agglutinates involves reduction of Fe in the target material to generate nm-scale spherules of metallic Fe (nanophase Fe0 or npFe0). The ratio of elemental Fe, in the form of npFe0, to FeO in a given bulk soil indicates its maturity, which increases with length of surface exposure as well as being typically higher in the finer-size fraction of soils. The melting and mixing process in agglutinate formation remain poorly understood. This includes incomplete knowledge regarding how the homogeneity and overall compositional trends of the agglutinate glass portions (agglutinitic glass) evolve with maturity. The aim of this study is to use sub-micrometer scale X-ray compositional mapping and image analysis to quantify the chemical homogeneity of agglutinitic glass, correlate its homogeneity to its parent soil maturity, and identify the principal chemical components contributing to the shock melt composition variations. An additional focus is to see if agglutinitic glass contains anomalously high Fe sub-micron scale compositional domains similar to those recently reported in glassy patina coatings on lunar rocks.

Vance, A. M.↗

NASA NTRS2012

Quasi-Monolithic Structures for Spaceflight Using Hydroxide-Catalysis Bonding

Future space-based missions will take measurements of the universe with unprecedented results. To do this, these missions will require materials and bonding techniques with ever-increasing stability in order to make their measurements. As an example, the Laser Interferometer Space Antenna (LISA) will detect and observe gravitational waves in the 0.1 mHz to 1 Hz frequency range with strain sensitivities on the order of 10(exp -21) at its most sensitive frequency. To make these measurements, critical components such as the optical bench or telescope support structure, will need to have path-length stabilities of better than 1 pm/(square root)Hz. The baseline construction method for the LISA optical bench is to affix fused silica optical components to a Zerodur baseplate using hydroxide-catalysis bonding (HCB). HCB is a recently developed technique that allows the bonding of glasses, some metals, and silicon carbide with significant strength and stability with a bond thickness of less than a few micrometers. In addition, a wide range of surface profiles can be bonded using only a small amount of hydroxide solution. These characteristics make HCB ideal for adhering optical components in complex optical systems. In addition to being used to construct the LISA optical bench, the HCB technique shows great promise for constructing other structures such as hollow retroreflectors to be used for lunar laser ranging, or a visible nulling coronograph to be used for exo-planet detection. Here we present construction techniques that could be used to make an optical bench, hollow retroreflector, nulling coronograph, or other quasi-monolithic structures using HCB. In addition, we present dimensional stability results of an optical bench that was made using HCB, as well as HCB strength measurements.

Preston, Alix↗

DOE OSTI2022

Effects of thin metal contacts on few-layer van der Waals ferrielectric CuInP 2 S 6

Out-of-plane polarized ferroelectric materials in a capacitive structure provide a key component for several technological applications. Furthermore, two-dimensional materials are expected to aid in the quest for both ultrathin and flexible electronics. Of the various two-dimensional ferroelectrics with out-of-plane polarization, CuInP 2 S 6 is special in that the Cu atoms are highly mobile and it has been shown to possess both low- and high-polarization states. Here, using density-functional-theory calculations, we explore the stabilization of the ferroelectric state for several prototypical metal contacts (Gr, Ni, Cu, Au, and Ag). In all cases, we find that the ferroelectric state can be stabilized at fewer layers than in the freestanding case. For all of the considered conventional metal contacts, we also find the existence of a quasi-ferroelectric state that stabilizes a polar phase for thicknesses greater than two layers of CIPS. In the cases of Au and Ag, interfacial alignment and strain can be used to stabilize ferroelectricity at the bilayer limit. Furthermore, we find that the strength of the interaction between the contact and CuInP 2 S 6 also leads to stabilization of the high-polarization state when ferroelectricity is stabilized. Lastly, energy-barrier calculations show that the system is still switchable in the presence of contact doping from the metal contacts.

2D materials↗

DOE OSTI2023

A lightweight and metal-free current collector for battery anode applications

The requirement for high energy density batteries is driving the development of high-capacity electrode materials while reducing the amount of inactive battery components such as separators, binders, and current collectors. Though current collectors are an inactive component, they are still required for successful working of a battery cell. Conventional current collectors include aluminum foil for cathode and copper foil for anode. Copper foil is quite heavy (8.7 mg/cm 2 ) for 10μm thickness. Therefore, there is a need for a lightweight current collector for anode applications. In this work, a metal-free current collector comprised of aligned carbon fiber (CFs) layer filled with carbon nanotubes (CNTs) mixed in polymer (P) is developed to be used as a current collector for anodes. Further, anodes coated on the CF-CNT-P showed lower charge transfer resistance and improved rate capability compared with the anodes fabricated on conventional copper foil-based current collectors. The CF-CNT-P are lighter (≈1.5 mg/cm 2 ) than the commonly used copper foil (8.7 mg/cm 2 ), which will increase the gravimetric energy density.

25 ENERGY STORAGE↗

DOE OSTI2019

Overview of Novel Canadian Approaches for Decontamination of Solid Radioactive and Mixed Waste - 19476

The availability of decontamination-for-release technology options provide a path forward to economically decontaminate radioactive metallic waste and enable its disposal as clean scrap metal, to decontaminate tools/equipment for unrestricted refurbishment or reuse, and to carry out inspection of in-service components. Projects involving management of solid mixed waste pose complex technical challenges that require the development and application of novel decontamination processes. The objective of this paper is to present project case studies that provide an overview of Kinectrics' experience with the decontamination of solid radioactive and mixed waste. Novel approaches to decontamination, recent developments, key results and lessons learned will also be discussed. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRSDate not supplied

Successes and Failures of Metal Additive Manufacturing for Rocket Engines

NASA has been developing additive manufacturing (AM) for various technical and programmatic advantages for complex rocket engine and aerospace components. This maturation has focused on various AM processes, new alloys, characterizing material properties, developing standards, producing demonstrator parts, and integrating AM hardware in liquid rocket engines through test-fail-fix cycles, as well as application and dissemination of lessons learned of the AM lifecycle. The importance of proper AM processing was made evident in the failure of a Laser Powder Bed Fusion (L-PBF) copper-alloy combustion chamber during a hot-fire test due to a degraded material quality. The hot-fire test aimed to demonstrate high duty cycle under a risk-tolerant development project, where consequences of component failure would be minimal. However, the unintentional component failure emphasized the necessity of robust material characterization and rigorous process control procedures for the safe use of AM components in critical applications. This presentation provides an overview of the development failure, a discussion on the evaluation of the failed chamber and supplemental chambers produced at the same time, a representative material samples that included intentional build witness lines, and a summary of the key results and recommendations from the evaluations. NASA continues to approach AM processes and designs with a level of risk and acceptance of failures that is appropriate for the project objectives, with the overall goal of safe implementation of AM technology and transferring AM technology into commercial space applications. This presentation with provide critical awareness to the community lessons learned on proper implementation of AM.

Additive Manufacturing↗

DOE OSTI2022

Self-Sensing, Stretchable, Active Circuit Arrays: Liquid Metal Paste as a Combination Interconnect and Strain Sensor

Stretchable electrical interconnects and substrate materials are increasingly used to create flexible and con-formable electronic systems for soft robotics, smart textiles, and wearable devices. Wires fabricated using composite or liquid conductive inks encapsulated in silicone enable high strain and are mechanically robust. The resistance of these inter-connects increases with strain, which can present challenges for power delivery and signaling among electronic components. However, this effect can be used directly to estimate strain within a stretchable circuit without the need for additional sensor components. In this work, we present an approach for fabricating fully-stretchable, multi-layer active circuit arrays in silicone using liquid metal paste interconnects, in which power and data wires are re-purposed as strain sensors to estimate substrate deformation. As a proof-of-principle, we demonstrate a 3×3 active circuit array that self-senses relative voltage supply at each node to estimate deformation and consumes less than 10 mA per node. Each node is digitally addressable and performs both analog measurement and digital conversion. All interconnects are fabricated using liquid metal paste, and power, data, and sensing are performed over a shared, four-wire interface in this multi-layer stretchable printed circuit board.

99 GENERAL AND MISCELLANEOUS↗

NASA NTRS1994

Compositional Variation in Apollo 16 Impact-Melt Breccias and Inferences for the Geology and Bombardment History of the Central Highlands of the Moon

High-precision data for the concentrations of a number of lithophile and siderophile elements were obtained on multiple subsamples from 109 impact-melt rocks and breccias (mostly crystalline) from the Apollo 16 site. Compositions of nearly all Apollo 16 melt rocks fall on one of two trends of increasing Sm concentration with increasing Sc concentration. The Eastern trend (lower Sm/Sc, Mg/Fe, and Sm/Yb ratios) consists of compositional groups 3 and 4 of previous classification schemes. These melt rocks are feldspathic, poor in incompatible and siderophile elements, and appear to have provenance in the Descartes formation to the east of the site. The Western trend (higher Sm/Sc. Mg/Fe, and Sm/ Yb ratios) consists of compositional groups 1 and 2. These relatively mafic, KREEP-bearing breccias are a major component (approx.35%) of the Cayley plains west of the site and are unusual, compared to otherwise similar melt breccias from other sites, in having high concentrations of Fe-Ni metal ( 1-2 %). The metal is the carrier of the low-Ir/Au (approx. 0.3 x chondritic) siderophile-element signature that is characteristic of the Apollo 16 site. Four compositionally distinct groups (1M, 1F, 2DB, and 2NR) of Western-trend melt breccias occur that are each represented by at least six samples. Compositional group 1 or previous classification schemes (the 'poikilitic' or 'LKFM' melt breccias) can be subdivided into two groups. Group 1M (represented by six samples, including 60315) is characterized by lower Al2O3 concentrations, higher MgO and alkali concentrations, and higher Mg/Fe and Cr/Sc ratios than group 1F (represented by fifteen samples, including 65015). Group 1M also has siderophile-element concentrations averaging about twice those of group lF and Ir/Au and Ir/Ni ratios that are even lower than those of other Western-trend melt rocks (Ir/Au = 0.24 +/- 0.03. CI-normalized). At the mafic extreme of group 2 ('VHA' melt breccias), the melt lithology occurring as clasts in feldspathic fragmental breccias from North Ray crater (group 2NR) is compositionally distinct from the melt lithology ofdimict breccias from the Cayley plains (group 2DB) in having higher concentrations of Sc, Cr, and heavy rare earth elements and lower concentrations of siderophile elements. The distinct siderophile-element signature (high absolute abundances, low Ir/Au ratio) suggest that the four groups ofmafic melt breccia are all somehow related. Ratios ofsome lithophile elements also suggest that they are more closely related to each other than then, are to melt breccias from other Apoll sites. However, none of the breccia compositions can be related to any of the others by any simple process of igneous fractionation or mixing involving common lunar materials. Thus, the origin of the four groups of mafic melt breccia is enigmatic. If they were produced in only one or two impacts, then a mechanism exists for generating regimes of impact-melt breccia in a single impact that are substantially different from each other in composition. For various reasons, including the problem of delivering large volumes of four different types of melt to the Apollo 16 site, it is unlikely that any of these breccias were produced in basin-forming impacts. If they were produced in as many as four crater-forming impacts, then the unusual siderophile-element signature is difficult to explain. Possible explanations are (1) the four groups of melt breccia all contain metal from a single, earlier impact, (2) they were each formed by related metal-rich meteoroids, or (3) some common postimpact process has resulted in metal of similar composition in each of four melt pools. Within a compositional group, most intrasample and intersample variation in lithophile element concentrations is caused by differences among samples in the proportion of a component of normative anorthosite or noritic anorthosite. In most cases, this compositional variation probably reflects variation in clast abundance. For group 2DB (and probably 2NR), differences in abundance of a component of ferroan anorthosite (estimated Al2O3 approx. 32%) accounts for the compositional variation. For groups 1M and 1F, the anorthositic component is more mafic (estimated Al203 approx. 26%). Some group-2 samples may be related by a troctolitic component of varying abundance.

Korotev, Randy L.↗

DOE OSTI2021

Two-Component Multireference Restricted Active Space Configuration Interaction for the Computation of L-Edge X-ray Absorption Spectra

X-ray absorption spectroscopy is a powerful probe of local electronic and nuclear structure, providing insights into chemical processes. The theoretical prediction and interpretation of metal L-edge X-ray absorption spectra is complicated by both relativistic effects, including spin-orbit coupling, and by the multiconfigurational nature of the states involved. This work details an exact two-component multireference restricted active space configuration interaction (X2C-MRRASCI) scheme that uses an exact two-component state average complete active space self-consistent-field method (X2C-SA-CASSCF), which includes the spin-orbit coupling in a variational manner, for the accurate description of the electronic structure before using a restricted active space configuration interaction method to describe the core excited states of the X-ray spectrum. Benchmark calculations are presented for a series of iron containing complexes, with results showing key features of the spectrum being reproduced, including ligand to metal charge transfer and shake-up excitations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Densification Pressure Optimization of MOF-808-Based Membranes for Lithium Metal Batteries

The use of metal–organic frameworks (MOFs) in hybrid electrolytes for lithium (Li) metal batteries has grown in prominence in recent years, primarily due to the chemical tunability of the MOF’s pore structures, which can directly influence Li–ion transport properties. The most attractive form factor for a MOF electrolyte is a thin, flexible membrane, which requires the application of pressure to increase the contact between the MOF particles. Herein, a systematic study of the influence of pressure on the properties of MOF-808-based membranes is presented. It is shown that when a dry, roll-pressed membrane is subjected to pressure ≥120 MPa, a total loss of crystallinity and a significant loss of porosity is observed. Alternatively, a slurry-cast membrane, compressed under controlled pressures, can maintain crystallinity and porosity while decreasing the interparticle void space. Interesting, the conductivity of the membranes infiltrated with liquid electrolyte is not greatly affected by the pressure applied, though ultimately it is shown that for cycling with Li metal, compressed membranes with compact particles are preferred. In conclusion, this study highlights the critical importance of controlling the pressure applied to MOF-based membranes during fabrication and during cell assembly and lays out the foundation for further investigation of how to optimize membrane fabrication for hybrid electrolytes that use MOFs as the dominate component.

25 ENERGY STORAGE↗

DOE OSTI2023

Effect of Ionic Strength and Anion Identity on Rare‐Earth Element Chelation by Poly(acrylic acid)

Abstract Rare‐earth elements (REEs) are critical components of many modern technologies, but their efficient separation and purification continue to pose significant challenges. Metal‐binding polymers may enable the development of promising alternative approaches to conventional separation techniques (e.g., solvent extraction), and insights into the interactions between the metal ions and polymers in solution are crucial to such development. In this work, the effect of ionic strength on the chelation of REEs by poly(acrylic acid) is investigated using isothermal titration calorimetry (ITC) to measure the metal‐binding thermodynamics. ITC experiments revealed that when ionic strength increases from increasing the sodium acetate buffer strength, polymer‐REE binding becomes increasingly disfavored. However, when ionic strength is increased by the addition of sodium chloride, binding again becomes increasingly disfavored, but to a lesser extent than when ionic strength increases from increasing the buffer strength. Additionally, the reduction in binding affinity is enthalpically driven when ionic strength is raised with sodium chloride, while it is entropically driven when raised with sodium acetate buffer, suggesting competive binding by the acetate ions. These results highlight the importance of ionic strength in polymer‐metal binding thermodynamics and will guide the development of new processes for the purification of critical metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Aluminum/SmCo 5 composites for structural and magnetic applications

Metal-bonded magnetic composites (MBMCs) present a promising alternative to dense sintered magnets, particularly for intricate components. Compared to polymer-based bonded magnets, MBMCs have wider applicability in harsh environments. In this paper, we demonstrate a solid-state shear-based manufacturing technique to introduce localized magnetization into a paramagnetic aluminum matrix by embedding SmCo5 permanent magnet particles. Our magnetic composites display hard magnetic behavior with a coercivity of 13 kOe and a remanent magnetization of 4.32 emu/g. In addition to magnetization, we also report a 9% improvement in Young’s modulus. Despite the local temperature rise during processing, the magnetic phases didn’t decompose into unwanted phases, preserving the composite's hard magnetic properties. Creation of an interfacial metallurgical bond with the matrix ensured the suitability of the composites for structural applications. Our study investigates the mechanical, and functional properties of composites, paving the way for lightweight structural magnetic composites with a transformative potential in the aerospace, nuclear, and automotive applications. This work underscores the potential for further optimization and development to drive innovations in magnet and equipment design.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Investigating sol–gel matrix loading capacity toward producing surrogate nuclear explosive debris with realistic composition

Post detonation nuclear forensic materials which resemble the size, color, elemental composition, and radionuclide content of real nuclear debris would be valuable for developing and validating new nuclear forensic techniques. As nuclear fallout types vary significantly, the ability to tailor each of these parameters accurately is desired to produce materials capable of testing analytical methods under a wide array of forensic scenarios. Sol–gel synthesis techniques can provide tunability of size, shape and composition for producing a wide variety of solid nuclear forensics benchmarking materials. Further, the sol–gel process consists of forming a metal oxide material, often silica, through polymerization of a metal-alkoxy precursor. In this work, we characterize the ability to load sol–gel particles with secondary elemental components such as iron, aluminum, and calcium toward producing benchmarking materials approximating the elemental composition of historic nuclear debris from the Nevada National Security Site. We also demonstrate quantitative radionuclide encapsulation toward producing benchmarking materials with controllable radionuclide content. Finally, we employ these techniques to produce nuclear debris benchmarking materials with controllable elemental matrix composition and radionuclide content and compare these samples with the composition of a historic fallout sample previously reported from the Nevada National Security Site.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Liquid lithium wetting and percolation in a porous tungsten/liquid Li plasma facing component (PFC)

This work explores the concept of a hybrid material system designed to protect the plasma from high-Z material emission while also protecting an underlying high-Z wall material from erosion by integrating a low-Z component in the liquid phase. Plasma-surface interaction properties of a porous tungsten (W)-liquid metal hybrid system, having the favorable bulk thermomechanical properties of W while serving as a scaffold for a liquid metal with self-healing and radiative vapor shielding characteristics, are examined. W-substrates with 70% density of bulk W and 1–5 μm sized pores have been fabricated with 50-nm W powders using spark plasma sintering. Enhanced lithium (Li) wettability, driven by percolation through the porous W architecture, is demonstrated with in-situ liquid Li drop measurements. Finally, results show complete wetting of liquid Li at 250 °C in the porous W, 100 °C lower temperature than what has been observed on traditional W surfaces. In operando ion beam analysis of Li films deposited on porous W substrates provides microscopic evidence of Li percolation into the substrate and a first look at D retention up to a depth of 100 nm after plasma exposure at a flux of 10 20 m –2 s –1 , 250 eV/amu D + plasma to a fluence of 1.16 × 10 23 m –2 at a temperature of 200 °C.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Exploring the Structure–Function Relationship in Iridium–Cobalt Oxide Catalyst for Oxygen Evolution Reaction across Different Electrolyte Media

Renewable hydrogen generation from water electrolysis offers a viable path to decarbonization if the costs can be reduced. The iridium-based anode catalyst is one of the most expensive components in electrolyzers. We propose reducing iridium usage by substituting Ir with Co, a more affordable metal, in the mixed oxide phase to enhance the catalytic activity while minimizing Ir consumption. A modified surfactant-assisted Adams fusion synthesis technique was developed as a scalable method for producing IrCo oxide nanoparticles. The synthesized material outperforms the commercial baseline, iridium oxide with carbon (IrOx_C), in both acidic and alkaline media. Acid etching (IrCo_ae) further enhances activity by selectively removing Co to expose more active sites. IrCo_ae achieved a significantly lower overpotential at 10 mA/cm 2 compared to IrOx_C, with reductions of approximately 18% under acidic conditions and 14% under alkaline conditions. This work demonstrates that the proposed synthesis method enables efficient Ir utilization and can be adapted to enhance catalyst stability for renewable hydrogen production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Inter-ligand cross-links determine secondary building unit formation in oligoMOFs

OligoMOFs are a class of metal–organic frameworks (MOFs) that feature ligands covalently cross-linked into oligomers as intrinsic structural components. A recent study has demonstrated that the size and flexibility of the tether moieties can result in the formation of oligoMOFs with different isomeric structures via geometrical distortions in the secondary building unit (SBU). In this work, it is demonstrated that tethered dimeric ligands with slightly different carbon chain lengths can direct the formation of oligoMOFs with SBUs of different structure and nuclearity. Specifically, inter-ligand cross links are used as a sensitive probe of the phase landscape of MOFs with the composition [Zn 2 (R-bdc) 2 (bpy)] (bdc = 1,4-benzenedicarboxylate, bpy = 4,4′-bipyridine), showing that a hexyl tether results in a framework structure identical to MOF-508, based on dinuclear {Zn 2 } “paddlewheel” SBUs, while heptyl and octyl tethers result in a “honeycomb-like” framework structure based on an infinite rod-like Zn 2+ SBU bridged by carboxylate ligands. Furthermore, these results are the first examples of tether length influencing SBU chemistry in MOFs and help understand the interplay between the MOF lattice and the geometric constraints imposed by inter-ligand cross-links in oligoMOFs.

MOFs↗