SEARCH · Engineering Papers

Results for “liquid solid interfaces”

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.

SourceResearch connectionFrom yearThrough year

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 145 records · Page 8

All sources NASA NTRS DOE OSTI

DOE OSTI2022

Microstructural pattern formation during liquid metal dealloying: Phase-field simulations and theoretical analyses

In recent years, liquid metal dealloying has emerged as a promising material processing method to generate micro- and nanoscale bicontinuous or porous structures. Most previous studies focused on the experimental characterization of the dealloying process and on the properties of the dealloyed materials, leaving the theoretical study incomplete to fully understand the fundamental mechanisms of the liquid metal dealloying process. In this paper, we use theoretical models and phase-field simulations to clarify the kinetics and pattern formation during liquid metal dealloying. Our investigation starts from a theoretical analysis of the 1D dissolution of a binary precursor alloy, which reveals that the 1D dissolution process involves two regimes. In the first regime, due to the low solubility of one of the elements in the melt, it accumulates at the solid-liquid interface, which reduces the dissolution kinetics. In the second regime, the interface kinetics reaches a stationary regime where both elements of the precursor alloy dissolve into the melt. Previous works revealed that in the early dealloying stage, the dealloying front is destabilized by an interfacial spinodal decomposition, which triggers the formation of interconnected ligaments. Here we extend this line of work by proposing a linear stability analysis able to predict the initial length scale of the ligaments formed in the initial stage of the dealloying. Combining this analysis with the 1D dissolution model proposed here enables us to better understand the initial conditions (composition of the precursor alloy and the melt) leading to a planar dissolution without interface destabilization. Finally, we report a strong influence of solid-state diffusion on dealloying. Although the solid-state diffusivity is four to five orders of magnitude smaller than in the liquid phase, it is found to affect both dissolution kinetics and ligament morphologies.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Ubiquitous short-range order in multi-principal element alloys

Recent research in multi-principal element alloys (MPEAs) has increasingly focused on the role of short-range order (SRO) on material performance. However, the mechanisms of SRO formation and its precise control remain elusive, limiting the progress of SRO engineering. Here, leveraging advanced additive manufacturing techniques that produce samples with a wide range of cooling rates (up to 10 7 K s –1 ) and an enhanced semi-quantitative electron microscopy method, we characterize SRO in three CoCrNi-based face-centered-cubic (FCC) MPEAs. Surprisingly, irrespective of the processing and thermal treatment history, all samples exhibit similar levels of SRO. Atomistic simulations reveal that during solidification, prevalent local chemical order arises in the liquid-solid interface (solidification front) even under the extreme cooling rate of 10 11 K s –1 . This phenomenon stems from the swift atomic diffusion in the supercooled liquid, which matches or even surpasses the rate of solidification. Therefore, SRO is an inherent characteristic of most FCC MPEAs, insensitive to variations in cooling rates and even annealing treatments typically available in experiments.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Charges on a suspended silicon nitride membrane under a high-energy electron beam

Thin silicon nitride (SiN x ) membranes are widely used in gas and liquid phase transmission electron microscopy (TEM) and as phase plates to enhance imaging contrast. SiN x contains trap sites for both positive and negative charges, which can be manipulated by high-energy electron irradiation, external potential biasing, or light exposure. Charge accumulation on the membrane can significantly affect in situ TEM processes, including chemical and electrochemical reactions, nanoparticle dynamics, and catalytic activity, or introduce unwanted phase shifts when used as a phase plate. Here, in this study, charge accumulation on suspended SiN x membranes was investigated using off-axis electron holography combined with model-free charge analysis, supported by custom finite element analysis (FEA) simulations. An average residual positive charge density of approximately 2.8 × 10 −4 C m −2 was measured. Localized and stable regions of both positive and negative charges were identified on the membrane. The global positive and localized positive/negative charges give rise to strong electric fields and electroosmotic slip velocities at the membrane surface, which are sufficient to induce non-Brownian particle behavior and directional fluid flow, offering a physical explanation for previously observed anomalies in particle dynamics, nucleation, and growth during gas and liquid phase TEM experiments. These results provide a benchmark for understanding charge behavior at SiNx interfaces in gas and liquid phase TEM. Furthermore, the FEA simulations establish a framework for future investigations into charge distribution, electrostatic potentials, and electrical double layers at solid–liquid interfaces, particularly in complex geometries and chemically dynamic environments.

Suspended silicon↗

NASA NTRS1990

Natural melting within a spherical shell

Fundamental heat transfer experiments were performed on the melting of a phase change medium in a spherical shell. Free expansion of the medium into a void space within the sphere was permitted. A step function temperature jump on the outer shell wall was imposed and the timewise evolution of the melting process and the position of the solid-liquid interface was photographically recorded. Numerical integration of the interface position data yielded information about the melted mass and the energy of melting. It was found that the rate of melting and the heat transfer were significantly affected by the movement of the solid medium to the base of the sphere due to gravity. The energy transfer associated with melting was substantially higher than that predicted by the conduction model. Furthermore, the radio of the measured values of sensible energy in the liquid melt to the energy of melting were nearly proportional to the Stefan number. The experimental results are in agreement with a theory set forth in an earlier paper.

Bahrami, Parviz A.↗

NASA NTRS2019

Intern Designed Modules for Conducting Potential Microgravity Solidification Experiments Aboard the International Space Station

MMaJIC (Microgravity Materials Joining Investigation Chamber) is a modular experiment chamber for performing materials science investigations. MMaJIC was initially designed to provide a controlled and sealed test environment to accommodate a wide variety of soldering and brazing experiments. However, its modular cartridge design is well suited to easily conduct any number and variety of science experiments. SoLIDD (Solid Liquid Interface Directional Device) is an apparatus for conducting directional solidification experiments with low melting temperature alloys. It has capability for varying the sample’s temperature gradient and growth velocity thus ensuring microstructural development under controlled conditions. ICED-T (Interface Control Experiment with Directional Translation) is an apparatus that conducts directional solidification experiments of transparent materials such that direct observation/recording of the advancing solid/liquid interface can be made. Currently, it is a functional breadboard that consists of the components mounted to a surface that allows the sample to be placed in an upright position. Orientation of the experiment (solid on the bottom, liquid on top) is important during testing ground samples to maintain stability. Ultimately, the goal of MMaJIC, SoLIDD and ICED-T is to conduct successful ground tests and then be re-configured for eventual use by aboard the ISS.

McElderry, Justin↗

NASA NTRS1999

Effect of Interface Shape and Magnetic Field on the Microstructure of Bulk Ge:Ga

Thermal and compositional gradients induced during the growth process contribute significantly to the development of defects in the solidified boule. Thermal gradients and the solid-liquid interface shape can be greatly effected by ampoule material. Compositional gradients are strongly influenced by interface curvature and convective flow in the liquid. Results of this investigation illustrate the combined influences of interface shape and convective fluid flow. An applied magnetic field was used to reduce the effects of convective fluid flow in the electrically conductive melt during directional solidification. Several 8 mm diameter boules of Ga-doped Ge were grown at different field strengths, up to 5 Tesla, in four different ampoule materials. Compositional profiles indicate mass transfer conditions ranged from completely mixed to diffusion controlled. The influence of convection in the melt on the developing crystal microstructure and defect density was investigated as a function of field strength and ampoule material. Chemical etching and electron backscattered electron diffraction were used to map the crystal structure of each boule along the center plane. Dislocation etch pit densities were measured for each boule. Results show the influence of magnetic field strength and ampoule material on overall crystal quality.

Cobb, S. D.↗

DOE OSTI2022

Heterogeneous phase transformation pathways in additively manufactured Al-Ce-Mn alloys

Heat treatment of additively manufactured Al-Ce based multicomponent alloys leads to complex microstructure evolution. In this research, the ability to extend the phase transformation theories involving nucleation of a product phase from a heterogeneous multi-phase microstructure typical to that of additively manufactured samples is explored. The Al-10Ce-8Mn (wt%) was used as a model alloy system. Under additive manufacturing conditions different solidification microstructures were obtained due to spatial and temporal variations of thermal gradients (G) and liquid-solid interface velocities (R) within a given melt pool. Near the melt pool boundary (high G and low R, referred as MPB region), initially, Al 20 Mn 2 Ce forms from the liquid followed by a eutectic of FCC Al and Al 11 Ce 3 . In the melt pool interiors (low G and high R referred as ES region) a eutectic structure between FCC Al and Al 20 Mn 2 Ce is observed. During subsequent heat treatments, the MPB and ES regions transform into different sets of microstructures. In the MPB region, a fine globular microstructure containing FCC Al, Al 11 Ce 3 , Al 6 Mn, and Al 12 Mn results from the decomposition of Al 20 Mn 2 Ce. In the ES region a faceted Al 51 Mn 7 Ce 4 plate phase results from the decomposition of Al 20 Mn 2 Ce. The formation of the Al 51 Mn 7 Ce 4 phase within the eutectic microstructure at the boundaries of FCC Al and Al 20 Mn 2 Ce has not been reported in the literature. Further, these two distinct phase transformation pathways are rationalized based on the role of driving force on the nucleation of (Al 6 Mn) and/or metastable intermetallic (Al 51 Mn 7 Ce 4 ) phases at the interface of aluminum (FCC) and the non-equilibrium intermetallic (Al 20 Mn 2 Ce) phases.

36 MATERIALS SCIENCE↗

NASA NTRS1986

Interaction of flows with the crystal-melt interface

The coupling between a crystal-melt interface and fluid flow is investigated. The solidification boundary conditions at the crystal-melt interface are described. The influences of morphological and double-diffusive instabilities during directional solidification on the interface are studied. The experiments by Glicksman and Mickalonis (1982) and Fang et al. (1985) which examine the relationship between the hydrodynamic state of the phase melt and phase-change interface are analyzed. The Rayleigh-Benard problem, and the effect of crystal-melt interaction on the Rayleigh number are examined. Various applications for melt-flow interactions with solid-liquid interface to engineering and welding are discussed.

Glicksman, M. E.↗

NASA NTRS1999

The Isothermal Dendritic Growth Experiment (IDGE): USMP-4 One-Year-Report

Dendrites describe the tree-like crystal morphology commonly assumed in many material systems--particularly in metals and alloys that freeze from supercooled or supersaturated melts. There remains a high level of engineering interest in dendritic solidification because of the role of dendrites in the determination of cast alloy microstructures. Microstructure plays a key role in determining the physical properties of cast or welded products. In addition, dendritic solidification provides an example of non-equilibrium physics and is one of the simplest non-trivial examples of dynamic pattern formation, where an amorphous melt, under simple starting conditions, evolves into a complex ramified microstructure. Although it is well-known that dendritic growth is controlled by the transport of latent heat from the moving solid-melt interface as the dendrite advances into a supercooled melt, an accurate, and predictive model has not been developed. Current theories consider: 1) the transfer of heat or solute from the solid-liquid interface into the melt, and 2) the interfacial crystal growth and growth selection physics for the interface. However, the effects of gravity-induced convection on the transfer of heat from the interface prevent either element from being adequately tested solely under terrestrial conditions. The Isothermal Dendritic Growth Experiment (IDGE) constituted a series of three NASA-supported microgravity experiments, all of which flew aboard the space shuttle, Columbia. This experimental space flight series was designed and operated to grow and record dendrite solidification in the absence of gravity-induced convective heat transfer, and thereby produce a wealth of benchmark-quality data for testing solidification scaling laws. The data collection from the on-orbit phase of the IDGE flight series is now complete. We are currently completing analyses and moving towards final data archiving.

Glicksman, M. E.↗

DOE OSTI2024

Cryogenic EM Across Length Scales for Li Metal Anode Batteries

An interfacial understanding is necessary for developing strategies to commercialize high-energy density rechargeable lithium metal anode batteries, as currently, the lithium anode/electrolyte interface is unstable with prolonged cycling. We have used several strategies to improve the cycling performance of lithium metal anodes, including reducing the parasitic reactions between lithium metal and the electrolyte, and improving the electrodeposited lithium metal morphology. These strategies have generated unconclusive electrochemical data, that has required the need for nanoscale interfacial characterization of these solid-liquid interfaces. Our team has used the cryogenic transfer workflow developed by Leica in collaboration with cryo-SEM/FIB tools by Thermo Fisher Scientific to cross-section lithium metal anodes and intact coin cell batteries to observe the interfacial structures, lithium morphology, and failure mechanisms relative to changes in electrode contract pressure and electrolyte chemistry. Cross-sectional SEM images and EDS maps of the lithium metal anodes have provided a better understanding of the electrodeposited lithium morphology, quantity of 'dead' lithium metal, and quantity of solid electrolyte interphase material that has formed alongside the lithium metal. In understanding lithium metal battery failure at the system level, we used a cryogenic stage in a laser plasma FIB to cross-section through the coin cell's cap for imaging/mapping the entire battery stack under cryogenic conditions. The tools, methods, and results of these studies will be detailed in this presentation.

characterization↗

DOE OSTI2025

Time-resolved electrical potential pump – X-ray photoelectron spectroscopy probe developments for investigating dynamic processes occurring at electrochemical interfaces

Electrode–electrolyte interfaces are of critical importance in several fields, including renewable energy, corrosion, and environmental chemistry. However, investigating these interfaces under operational conditions poses considerable challenges due to the limitations of the instrumentation employed. While recent advancements in in situ and operando techniques have enhanced our comprehension of the steady-state properties of solid-liquid interfaces, the dynamic behaviors of these systems remain inadequately explored. This study introduces a time-resolved X-ray photoelectron spectroscopy (XPS) technique designed to capture transient reaction intermediates and charging dynamics at electrified interfaces. The presented proof-of-principle study demonstrates that electrochemical processes, represented by an equivalent electrical circuit (EEC) model, can be probed and understood using square wave voltage pulses of a potentiostat synchronized to the modified data acquisition of an XPS setup. This method offers a valuable alternative to traditional pump–probe techniques, facilitating the investigation of a broader range of electrochemical systems. A dedicated software package for analyzing time- and energy-resolved XPS with a focus on extracting parameters of the EEC is geared towards benchmarking different EECs in future real-world electrochemical experiments.

Electrochemistry↗

NASA NTRS1985

Mephisto: Interfacial Destabilization in Metal Alloys

The destabilizing mechanisms at a solidification interface were studied to obtain information on the kinetics and morphologies in the transient and steady state, and to separate the influences of liquid phase instabilities from interfacial instabilities. A differential seebeck voltage measurements technique was developed to provide a continuous record of the solid-liquid interface temperature as the solidification rate is varied to determine the kinetic coefficients. Signal processing and noise suppression techniques allow nonovolt precision which corresponds to mK accuracy for the interfacial temperature.

Favier, J. J.↗

NASA NTRS1988

Dendritic growth of undercooled nickel-tin. III

The paper is concerned with structures and microsegregations in undercooled droplets of Ni-25 wt pct Sn and eutectic Ni-32.5 wt pct Sn alloys. An analysis of experimental results suggests that all samples solidify dendritically and that the final structures are largely the result of ripening. Experimental data on minimum solute composition in the samples produced are bounded by two curves both of which assume equilibrium at all liquid-solid interfaces during recalescence and subsequent cooling. The eutectic alloy samples often show a dendritic structure over the surface in areas where shrinkage is present. This structure appears to be the remnant of an original growth structure in which only limited ripening occurred, due to the rapid removal of interdendritic liquid by shrinkage.

Wu, Y.↗

NASA NTRS2000

Float-Zone Growth of Gel-xSix (x ? 10 at .%) Single Crystals: Influence of Thermocapillary and Solutocapillary Convection

Gel-xSix (x ? 10 at.%) single crystals have been grown with the float-zone technique applied within a monoellipsoid mirror furnace. The feed crystal consisted of synthesized GeO.95siO.05 polycrystalline material. Two Boron-doped (much much more than 1-2 (raised dot) 1017 at/cm3) crystals were grown under identical conditions using <100> Ge seeds. One Ge:Ga-doped (much much more than 1018 at/cm3) reference crystal was also grown in the same furnace. Compositional profiles were measured with an energy dispersive analysis by X-ray (EDAX). The maximum silicon concentration attained was 10 at.%. Micrographs of the etched crystals show sharp changes in interface curvature at the crystal edges. These are considered to be caused by solutal Marangoni convection, whose strength is assumed to be a direct function of silicon concentration, Theoretical considerations show that the flow direction, velocity, and strength varies significantly from a solutal Marangoni convection regime directly in front of the solid-liquid interface to a thermal Marangoni convection regime within the bulk melt.

Campbell, Tom A.↗

NASA NTRS1993

Laser-enhanced synthesis and processing of diamond films from liquid hydrocarbons

We report synthesis of diamond films by pulsed laser irradiation on copper substrate immersed into liquid benzene. It is envisaged that carbon released from benzene at the liquid-solid interface is converted into diamond as a result of rapid quenching from a high temperature. The diamond crystallites were characterized using high resolution transmission electron microscopy imaging and electron diffraction techniques. Growth of thicker diamond films by subsequent chemical vapor deposition has been investigated by transmission and scanning electron microscopy techniques. Thin diamond film deposited during liquid phase provided seed for diamond growth during subsequent chemical vapor deposition.

Singh, Jogender↗

DOE OSTI2025

Methodology of Atomic Force Microscopy Visualization of Electrode–Electrolyte Interfaces

Electrochemical atomic force microscopy (EC-AFM) provides unprecedented insights into the microstructure of electrode–electrolyte interfaces during electrochemical reactions. However, performing EC-AFM measurements has many challenges, for example, drift, contamination, and probe degradation. We present solutions to these experimental issues through electrochemical cell design and carefully chosen experimental parameters. The possibility that the probes can react with the interface during scanning, generating false-positive electrochemical dynamics, is discussed as an example of the challenge of high-fidelity EC-AFM measurement. Here, we demonstrate this effect in highly ordered pyrolytic graphite and show that we could use electrochemical control of the AFM probe to enable high-fidelity in situ AFM visualization of solid–liquid interfaces during electrochemical reactions.

Electrochemical cells↗

DOE OSTI2023

Understanding In-Situ Structure and Chemistry at Battery Interfaces Through Time-Resolved Cryo-EM

Transmission and scanning transmission electron microscopy are vital tools for characterizing interfacial structure and chemistry at high spatial resolutions but are limited by the fact that many materials are quickly damaged by electron beam irradiation. This is a challenge particularly for materials relevant to energy applications, such as lithium-containing battery materials, organic-inorganic hybrids, and liquid electrolytes. Cryogenic electron microscopy (cryo-EM) offers a partial solution to this issue by stabilizing beam-sensitive solid-solid or solid-liquid interfaces for characterization, but typical cryo-EM sample preparations are ex situ and thus cannot capture interfaces in their electrified state of interest to applications. Here, we present a method to prepare cryo-EM samples of electrified battery interfaces in situ to preserve the time-resolved structures and chemistry that arise under applied current or bias.

batteries↗

DOE OSTI2022

Assessing entropy for catalytic processes at complex reactive interfaces

When chemical reactions are accelerated by a catalyst, entropy differences between reactants and their transient intermediates can be the driving force behind the promotion or inhibition of desired and parasitic chemical pathways. Understanding and controlling catalytic processes therefore requires both a fundamental and practicable understanding of entropy in addition to enthalpy. In unstructured media such as the vapor phase equilibrated with sparsely covered surfaces, entropy can be adequately accounted for by well-established approaches based on translational, rotational, and harmonic vibrational partition functions. However, these approximations become inadequate in more complex condensed phase environments, e.g., solid liquid interfaces of confined reaction spaces. In this chapter, we provide an overview of the state-of-art in the computational quantification of entropy and its known ramifications on catalysis. The fundamental roles of thermodynamics and kinetics in catalysis are covered in enough detail to appreciate and contextualize the computational methods employed to compute chemically accurate estimates of entropy. These methods are discussed in appropriate detail and range from the ubiquitous harmonic oscillator approximation where entropy unrelated to high frequency oscillations is typically underestimated, to enhanced free energy sampling with molecular dynamics where the desired accuracy must be weighed against the associated computational cost of obtaining it. The rising importance of machine learning and artificial intelligence in accelerating methodological progress in this field is touched upon, as well. Finally, applications, successes, and pitfalls of using these methods are provided to showcase past and present accomplishments while clarifying where improvements in both understanding and methodology are still needed.

Kollias, Loukas↗