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At least 721 records · Page 40
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Investigation of residual stress distribution in wire-arc directed energy deposited refractory molybdenum alloy utilizing numerical thermo-mechanical analysis and neutron diffraction method

Directed energy deposition (DED), a metal additive manufacturing (AM) technique, offers higher deposition rates and energy efficiency, making it suitable for fabricating components from refractory molybdenum alloys, such as molybdenum-titanium-zirconium (TZM). However, large thermal gradients and non-equilibrium thermal cycles in DED could generate high residual stress in the component, potentially deteriorating quality and performance. Thus, this study aims to investigate residual stress generation and its distribution in wire-arc DED of TZM thin-wall, utilizing thermo-mechanical analysis and high-fidelity neutron diffraction (ND) method. Two interpass temperatures (50°C and 200°C) have been considered to investigate their impact on residual stress formation. During experiments, in-situ thermal data has been recorded using thermocouples, which have been utilized for calibrating the thermal model. Thermocouple data shows a good agreement with the simulation results, having a difference of less than 10 %. Post-deposition part deformation has been observed, which is measured using a coordinate measuring machine, showing maximum values of 0.93 mm and 0.78 mm for interpass temperatures of 50°C and 200°C, respectively. Numerical predictions of distortion deviated by less than 15% from the experimental results. ND measurement and simulation results indicate that residual stress magnitude and evolution vary across the TZM deposits, revealing microstructural anisotropy in both conditions. Notably, lower interpass temperatures resulted in higher residual stresses, confirmed by experimental and simulation data. Further, this study demonstrated that an integrated experimental and thermo-mechanical analysis can potentially reveal the temperature history, part deformation, and residual stress formation in wire-arc DED TZM alloy.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Optimized Photoemission from Organic Molecules in 2D Layered Halide Perovskites

In recent years, hybrid organic−inorganic metal halides have been at the forefront of materials research. Typically, the functional (e.g., optoelectronic) properties of hybrid halides are derived from the inorganic structural part, whereas the organic structural units can add extra advantages in terms of stability, rigidity, and processability. Here, we report the design, synthesis, and characterization of two new hybrid materials in which the outstanding photophysical properties originate from the organic structural part. The new compounds, (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , have 2D layered Ruddlesden−Poppertype perovskite structures. These hybrids are blue-white light emitters just like their corresponding pure organic salts, but with much improved emission efficiencies. Optical spectroscopy and density functional theory (DFT) studies confirm that photoemission comes from the trans-stilbene organic cations. The photoluminescence quantum yield (PLQY) values of these new materials are among the highest known, 50.83% and 26.60% for (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , respectively. This is up to a 5-fold increase as compared to the light emission efficiency of the precursor salt C 15 H 16 NCl (PLQY of 10.33%). Alongside their outstanding optical properties, their environmental and thermal stability allow their consideration for potential practical applications such as radiation detection. This work shows that hybrid metal halides can be compositionally and structurally engineered to have highly efficient photoemission originating from the organic components for fast scintillation applications.

Halogens↗
DOE OSTI2020

Ultralight and fire-extinguishing current collectors for high-energy and high-safety lithium-ion batteries

Inactive components and safety hazards are two critical challenges in realizing high-energy lithium-ion batteries. Metal foil current collectors with high density are typically an integrated part of lithium-ion batteries yet deliver no capacity. Meanwhile, high-energy batteries can entail increased fire safety issues. Here we report a composite current collector design that simultaneously minimizes the ‘dead weight’ within the cell and improves fire safety. An ultralight polyimide-based current collector (9 μm thick, specific mass 1.54 mg cm-2) is prepared by sandwiching a polyimide embedded with triphenyl phosphate flame retardant between two superthin Cu layers (~500 nm). Compared to lithium-ion batteries assembled with the thinnest commercial metal foil current collectors (~6 µm), batteries equipped with our composite current collectors can realize a 16-26% improvement in specific energy and rapidly self-extinguish fires under extreme conditions such as short circuits and thermal runaway.

25 ENERGY STORAGE↗
DOE OSTI2026

Nanoengineering of non-aqueous liquid electrolyte solutions for future lithium metal batteries

Research and development of non-aqueous electrolyte solutions are essential for practical advancement towards the production of high-energy lithium metal batteries (LMBs). An ideal LMB electrolyte solution should enable highly efficient, uniform and prolonged lithium metal plating and stripping, preserve the electrodes’ electro(chemo)mechanical properties and ensure compatibility with all cell components. However, despite extensive research efforts, scientists have yet to achieve an electrolyte design that meets these requirements simultaneously. Here, by examining the nanoengineering aspects of various non-aqueous electrolyte solution designs, we elucidate the understanding of the nanoscale physicochemical and electrochemical processes taking place in LMBs, which are mainly governed by the thermodynamic and kinetic properties of the electrolyte system. We also explore emerging research directions and propose an accelerated, iterative framework that integrates nanoengineering principles with machine learning, high-throughput computation and experimentation to facilitate the development of next-generation non-aqueous electrolyte solutions for practical LMBs.

Weintz, Dominik↗
DOE OSTI2020

A review of composite solid-state electrolytes for lithium batteries: fundamentals, key materials and advanced structures

All-solid-state lithium ion batteries (ASSLBs) are considered next-generation devices for energy storage due to their advantages in safety and potentially high energy density. As the key component in ASSLBs, solid-state electrolytes (SSEs) with non-flammability and good adaptability to lithium metal anodes have attracted extensive attention in recent years. Among the current SSEs, composite solid-state electrolytes (CSSEs) with multiple phases have greater flexibility to customize and combine the advantages of single-phase electrolytes, which have been widely investigated recently and regarded as promising candidates for commercial ASSLBs. Based on existing investigations, herein, we present a comprehensive overview of the recent developments in CSSEs. Initially, we introduce the historical development from solid-state ionic conductors to CSSEs, and then summarize the fundamentals including mechanisms of lithium ion transport, key evaluation parameters, design principles, and key materials. Finally, four main types of advanced structures for CSSEs are classified and highlighted according to the recent progress. Moreover, advanced characterization and computational simulation techniques including machine learning are reviewed for the first time, and the main challenges and perspectives of CSSEs are also provided for their future development.

25 ENERGY STORAGE↗
DOE OSTI2023

Binding of carboxylate and water to monovalent cations

The interactions of carboxylate anions with water and cations are important for a wide variety of systems, both biological and synthetic. Here, in order to gain insight on properties of the local complexes, we apply density functional theory, to treat the complex electrostatic interactions, and investigate mixtures with varied numbers of carboxylate anions (acetate) and waters binding to monovalent cations, Li + , Na + and K + . The optimal structure with overall lowest free energy contains two acetates and two waters such that the cation is four-fold coordinated, similar to structures found earlier for pure water or pure carboxylate ligands. More generally, the complexes with two acetates have the lowest free energy. In transitioning from the overall optimal state, exchanging an acetate for water has a lower free energy barrier than exchanging water for an acetate. In most cases, the carboxylates are monodentate and in the first solvation shell. As water is added to the system, hydrogen bonding between waters and carboxylate O atoms further stabilizes monodentate structures. These structures, which have strong electrostatic interactions that involve hydrogen bonds of varying strength, are significantly polarized, with ChelpG partial charges that vary substantially as the bonding geometry varies. Overall, these results emphasize the increasing importance of water as a component of binding sites as the number of ligands increases, thus affecting the preferential solvation of specific metal ions and clarifying Hofmeister effects. Finally, structural analysis correlated with free energy analysis supports the idea that binding to more than the preferred number of carboxylates under architectural constraints are a key to ion transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Tailoring Corrosion Resistance of Additively Manufactured Metals with Atomic Layer Deposition

The goal of this work is to develop a scalable post-manufacturing capability at LANL that utilizes atomic layer deposition (ALD) for corrosion-resistant coatings onto additively manufactured (AM) metals. This will provide fundamentally new and essential capabilities towards the interchangeability of AM metals with traditionally wrought or machined material. This will be accomplished by (1) formulating novel ALD precursor doses and film thicknesses onto as-printed coupons of AM metals and (2) providing electrochemical characterization of corrosion susceptibility as a function of deposited film thickness. While ALD is well-established, the unique aspect (risk) of this work is application to rough AM surfaces. This risk is mitigated by repeating ALD deposition cycles, where thicker coatings laterally branch, resulting in a uniform coating. This risk will be assessed in the phase 1 feasibility study, wherein the application of ALD coatings to small AM coupon surfaces will be demonstrated using existing hardware and characterization tools at Sigma. This study alone will provide ground-breaking insight on the compatibility of ALD coating techniques with AM metals. Going beyond the phase 1 study, a standalone deposition chamber will be built, so full AM components can be coated and tested. While this MFR investment is focused on corrosion mitigation, it is critical to highlight external benefits of this technique outside the scope of this proposed study. ALD has extraordinary universality, whereby almost any material can be given almost any coating or graded density coating with atomic precision; and, the only limiting factors to scalability is the size of the dosing chamber. The self-limiting reactions intrinsic to ALD offers high conformity to part geometry and tolerance, even for internal surfaces where electroplating or conventional chemical vapor deposition falls short due to differential diffusion. This uniquely positions ALD at the forefront of post-manufacturing strategies for AM components, especially for those with complex geometry and internal surfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Progress Report of Alloy 709 Performance in Liquid Sodium

With improved high-temperature properties, Alloy 709 shows great potential for advanced reactor applications. To understand the effects of sodium on A709, small tensile specimens were machined from two commercial heats and subject to sodium exposure in two forced convection loops operated by Argonne. Thermal aging experiments were also conducted in parallel to isolate any sodium-specific effects. An increasing trend in yield strength and a decrease trend in ultimate tensile strength can be seen with the increasing exposure time, suggesting microstructural changes at these temperatures. Nonetheless, the thermally aged and sodium exposed samples behaved similarly, implying no sodium-specific effect at these temperatures. In contrast, 316H SS exposed to sodium at 650°C showed a strong sodium effect. The different responses of A709 and 316H SS to sodium exposure is of interest and requires additional effort to understand. The cold traps of the sodium loop were replaced early in FY23. During a maintenance operation, an unexpected sodium leak incident occurred at one of the sodium loops, triggering an emergency response. An investigation into the incident revealed that the leak happened at a VCR fitting on the recently replaced cold trap. The metal gasket of the leaked VCR fitting was not compressed sufficiently. A dimensional mismatch between the new component and old piping configuration was responsible for a significant misalignment. A new cold trap with improved design is in production. The new design provides additional flexibility and an access point for post-installation helium leak check and for venting of trapped gas. These design features will make the system more error-tolerant and the installation quality verifiable. A thermodynamic analysis was performed to understand the carburization-decarburization behavior of A709 in sodium environment. The equilibrium carbon activity in the alloy was evaluated with M 23 C 6 , TiC, and NbC. The carburization-decarburization boundary was calculated with different methods developed previously. The results suggests that A709 will be carburized in SMT-1 and SMT-2, and can be decarburized in low-carbon-activity environments such as EBR-II at temperatures above 620-650°C. Nonetheless, A709 should be less likely to be decarburized than 316H SS when exposed to the same low-carbon-activity environment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Demonstration of the surveillance test article for an advanced reactor surveillance test program

Operational environments in generation IV reactors involve corrosive and irradiative conditions at elevated temperatures. Typical reactor operations consist of transients which impose cyclic loads on reactor components. These cyclic loads, combined with corrosive and irradiative environments, result in synergistic degradation of component materials. However, limited data exists on the coupled damage effects on materials for reactor environments. While the surrogate material surveillance concept has been used in light water reactors to assess irradiation damage, existing material surveillance technologies are not suitable for in-situ monitoring of coupled material degradation. The materials surveillance program focuses on material degradation management and the estimation of remaining life of reactor components through surveillance test articles. This paper presents the design and analysis methodology of a bi-metal surveillance test article, which uses difference in thermal expansion coefficient between two metals to induce in-situ cyclic loads. This report presents the work conducted in FY 25, to test the surveillance test article in air and salt environments. These test specimens were evaluated after thermal cycle exposure and remaining life is measured through creep test.

36 - MATERIALS SCIENCE↗
DOE OSTI2020

Understanding and Strategies for Controlled Interfacial Phenomena in Lithium-Ion Batteries and Beyond

Electrolyte chemistry and properties and electrode structure and chemical properties particularly at the interfaces are crucial for the development of advanced battery components. This project focused on elucidating the roles of the electrolyte and electrode on the formation and evolution of the SEI layer and cell electrochemical performance on silicon and on Li metal anodes. For Si nano/microstructures we evaluated lithiation, volume changes, reactivity, and chemo-mechanical transformations as functions of nanoparticle size, shape, presence of coatings, electrolyte composition, electron leakage to the electrolyte, and cycling. For Li metal anodes we provided detailed analyses of the electrode and electrolyte effects on interfacial reactivity and as a function of microstructural evolution and underlying stochasticity as dendrites nucleate and grow. We thoroughly investigated and simulated how the chemistry of the various components of the electrolyte and the electrode architecture may affect the electrochemical reactions as well as cell degradation. A multiscale modeling approach was utilized, where atomistic simulations informed about the microscopic behavior of the system, and intermediate time and length scales were investigated with mesoscopic models. Results were also tested against selected experiments from our collaborators. The combined theoretical-experimental strategy saves costs by utilizing predictions from computational analyses to guide experimentation.

25 ENERGY STORAGE↗
DOE OSTI2026

Development of MOSCATO: A CFD-Level Electrochemistry and Corrosion Simulator for Molten Salt Systems

For both coolant and fueled variants of molten salt reactors (MSRs), the corrosion of structural materials is a significant challenge. The corrosion stems from chemical and electrochemical reactions initiated by fissile material, fission products, and impurities in the salt. Lower-fidelity models rely on empirical correlations for mass transfer, simplified lumped temperature profiles, and similar assumptions. They do not capture detailed spatial variations in complex geometries, creating the need for high-fidelity modeling to bridge this gap.As we approach the demonstration and possible deployment of MSRs in this decade, the development of a high-fidelity, high-performance simulator becomes imperative. To simulate the complex electrochemical environment and corrosion within molten salt systems, we have developed the Molten Salt Chemistry And TranspOrt (MOSCATO) code. This endeavor is comprised of three essential components. First, mass transfer equations are coupled with the Navier-Stokes equations in order to account for the transport of species in the salt. Second, the diffusion of alloy constituents, such as Cr, Fe, Ni, etc. is simulated within the structural metals. Third, the alloy and salt domains are coupled to account for the heterogeneous chemical and electrochemical reactions that occur at the salt-alloy interface.MOSCATO manages all three components within the framework of the highly scalable, open-source spectral element method computational fluid dynamics code Nek5000/NekRS. This integration enables MOSCATO to harness the immense computational power of modern high-performance computing resources, ensuring both high fidelity and computational speed.In addition to code development, we have initiated a comprehensive verification and validation campaign, utilizing data from diverse sources. First, MOSCATO's electrochemical solver was verified with reference numerical data. Then validation occurred against experiments: one of a thermal galvanic cell and the other for corrosion in flowing molten salt of FLiNaK (LiF-NaF-KF). This campaign verified and validated MOSCATO as a reliable tool for simulating electrochemical environments and corrosion in molten salt systems.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Technical Documents for Gateway for Accelerated Innovation in Nuclear (GAIN)

The Gateway for Accelerated Innovation in Nuclear (GAIN) provides the nuclear energy community with access to the technical, regulatory, and financial support necessary to move new or advanced nuclear reactor designs toward commercialization. GAIN provides the nuclear community with a single point of access to the broad range of capabilities (i.e., people, facilities, materials, and data) across the U.S. Department of Energy (DOE) complex and its National Lab capabilities. The Fast Flux Test Facility (FFTF) is the most recent liquid metal reactor (LMR) to be designed, constructed, and operated by DOE. The 400-MWt sodium-cooled, fast-neutron flux reactor plant was designed for irradiation testing of nuclear reactor fuels and materials for liquid metal fast breeder reactors. Following the demise of the breeder reactor program in the United States, FFTF continued to play a key role in providing a test bed for demonstrating performance of advanced fuel designs and demonstrating operation, maintenance, and safety of advanced liquid metal reactors. The FFTF Program provides valuable information for potential follow-on reactor projects in the areas of plant system and component design, component fabrication, fuel design and performance, reactor control, prototype testing, and site construction. This report provides documents related to three important aspects of FFTF design and operation: 1) irradiation behavior of structural alloys and absorber materials, 2) thermohydraulics of rod bundles (i.e., coolant mixing), and 3) natural circulation heat transfer in the areas of modeling and validation. These technical documents are believed to be of interest to the nuclear industry and in particular to designers of new liquid metal reactors.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2022

Toward Metal-free Photocatalysis: Photochemical Regeneration of Organic Hydride Donors Using Phenazine-Based Photosensitizers

Earth-abundant chromophores and catalysts are important molecular building blocks for artificial photosynthesis applications. Our team previously reported that metal-free hydride donors, such as biomimetic benzoimidazole-based motifs, can reduce CO 2 selectively to the formate ion and that they can be electrochemically regenerated using the proton-coupled mechanism. To enable direct utilization of solar energy, we report here the photochemical regeneration of a benzoimidazole-based hydride donor using a phenazine-based metal-free chromophore. The photochemical regeneration was investigated under different experimental conditions involving varying sacrificial donors, proton donors, solvents, and component concentrations. The best hydride regeneration yield of 50% was obtained with phenol as a proton source and thiophenolate as a sacrificial electron donor. The mechanism of photochemical regeneration was studied using steady-state and time-resolved UV/Vis spectroscopies. Based on the results of these studies, we hypothesize that the initial photoinduced electron transfer from photoexcited phenazine chromophores involves the benzoimidazole cation and that this process is likely coupled with proton transfer to generate protonated benzoimidazole-based radical cation. The second photoinduced electron transfer is hypothesized to generate the hydride form. Furthermore, our findings provide the requisite information for the future development of reductive photocatalysts for solar energy and light-harvesting applications utilizing earth-abundant metal-free materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Anode Upcycling via Tailored Solvent Treatment

To achieve a truly closed-loop direct recycling process for lithium-ion batteries, all component materials must be recovered. To date, direct recycling method development has primarily focused on the high-value transition-metal cathode materials, while the inherently lower-value graphite has been challenging to recover in a cost-effective manner. However, end-of-life graphite contains a unique engineered value due to the presence of the solid electrolyte interphase (SEI). Growth of the SEI during the cell's active lifetime stabilizes the electronically reactive graphite surface through an irreversible consumption of Li, and thus necessitates both excess lithiation of the cathode and a costly and time-intensive formation procedure during manufacturing. An optimized pre-formed SEI that capitalizes on existing SEI components from end-of-life batteries has the potential to significantly reduce cathode lithiation requirements and eliminate the critical bottleneck of formation cycling during cell remanufacturing. Further, retaining Li at the anode obviates the need for a separate Li leaching and recovery step, improving the overall efficiency of the direct recycling line. In this work, we present a novel approach to "upcycling" spent graphite through use of tailored chemical treatment to remove adverse (i.e., highly resistive and/or poorly passivating) SEI species while retaining beneficially passivating components. We have explored a rational set of solvents spanning a range of polarity, proticity, and molecular size to evaluate structure-property-performance relationships between applied solvent(s), removed and remaining SEI species, and electrochemical response of the resulting graphite product. Further, we have developed and optimized a robust and holistic analysis procedure that couples symmetric-cell electrochemical testing, multi-modal materials characterization, and advanced electrochemical modeling. These analysis results inform a set of correlative metrics for graphite performance relative to both solvent properties and upcycled SEI composition. We demonstrate effective tunability in the residual SEI composition by varying solvent identity and concentration, and report on several promising solvent systems that achieve comparable or performance to pristine graphite.

anode recycling↗
DOE OSTI2021

Electron shuttle in the MOF derived TiO 2 /CuO heterojunction boosts light driven hydrogen evolution

Metal organic frameworks (MOFs) have emerged as a novel template to develop porous photocatalytic materials for solar fuel conversion. In this work, we report the synthesis, charge separation dynamics, and photocatalytic performance of the TiO 2 /CuO heterostructure derived from mixed-phase MOFs based on Ti and Cu metal nodes, which demonstrates significantly enhanced catalytic activity for the hydrogen evolution reaction (HER) compared to metal oxides derived from single node MOFs. More importantly, using transient absorption spectroscopy, we identified the specific role each component in the heterostructure plays and unravelled the key intermediate species that is responsible for the exceptional photocatalytic activity of the heterostructure. We found that the HER is initiated with ultrafast electron transfer (<150 fs) from the molecular photosensitizer to the conduction band of TiO 2 , where TiO 2 acts as an electron mediator and shuttles the electron to the CuO cocatalyst, facilitating charge separation and ultimately boosting the HER efficiency. Overall, these results not only demonstrate the great potential of using mixed-phase MOFs as templates to synthesize mesoporous heterostructure photocatalysts but also provide important insight into the HER mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Axon-like active signal transmission

Any electrical signal propagating in a metallic conductor loses amplitude due to the natural resistance of the metal. Compensating for such losses presently requires repeatedly breaking the conductor and interposing amplifiers that consume and regenerate the signal. This century-old primitive severely constrains the design and performance of modern interconnect-dense chips. Here we present a fundamentally different primitive based on semi-stable edge of chaos (EOC), a long-theorized but experimentally elusive regime that underlies active (self-amplifying) transmission in biological axons. By electrically accessing the spin crossover in LaCoO 3 , we isolate semi-stable EOC, characterized by small-signal negative resistance and amplification of perturbations. In a metallic line atop a medium biased at EOC, a signal input at one end exits the other end amplified, without passing through a separate amplifying component. While superficially resembling superconductivity, active transmission offers controllably amplified time-varying small-signal propagation at normal temperature and pressure, but requires an electrically energized EOC medium. Operando thermal mapping reveals the mechanism of amplification—bias energy of the EOC medium, instead of fully dissipating as heat, is partly used to amplify signals in the metallic line, thereby enabling spatially continuous active transmission, which could transform the design and performance of complex electronic chips.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

Reduced Precious Metal Catalysts for CH 4 and NO x Emission Control of Natural Gas Vehicles

The abundant domestic natural gas resources coupled with the desire for clean air and reduced greenhouse gas emissions motivates the accelerated development of natural gas vehicles (NGVs) and engine. Methane (CH 4 ), a potent greenhouse gas, is the major component of natural gas. The current emission catalysts fall short in meeting the desired exhaust CH 4 emission standards for NGVs. In this project we have developed a class of novel Platinum Group Metal (PGM) basedmonolith catalysts with enhanced activity.

03 NATURAL GAS↗
DOE OSTI2023

A fluorinated cation introduces new interphasial chemistries to enable high-voltage lithium metal batteries

Abstract Fluorides have been identified as a key ingredient in interphases supporting aggressive battery chemistries. While the precursor for these fluorides must be pre-stored in electrolyte components and only delivered at extreme potentials, the chemical source of fluorine so far has been confined to either negatively-charge anions or fluorinated molecules, whose presence in the inner-Helmholtz layer of electrodes, and consequently their contribution to the interphasial chemistry, is restricted. To pre-store fluorine source on positive-charged species, here we show a cation that carries fluorine in its structure is synthesized and its contribution to interphasial chemistry is explored for the very first time. An electrolyte carrying fluorine in both cation and anion brings unprecedented interphasial chemistries that translate into superior battery performance of a lithium-metal battery, including high Coulombic efficiency of up to 99.98%, and Li 0 -dendrite prevention for 900 hours. The significance of this fluorinated cation undoubtedly extends to other advanced battery systems beyond lithium, all of which universally require kinetic protection of highly fluorinated interphases.

25 ENERGY STORAGE↗