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At least 37 records · Page 2

Role of electrolyte in silicon electrolyte interface stabilization

Transition metal ion dissolution was long thought to be the reason for poor cycling performance in Lithium ion batteries cycled to a high voltage, but since the anode SEI is electrochemically insulating, the mechanism for transition metal mediated SEI decomposition in unclear. Our results show that acidic species such as F 2 PO 2 H generation on the cathode side and their subsequent crossover reactions with the SEI components damaging it could more likely be a major factor to capacity fade.

25 ENERGY STORAGE↗

Interface stability in a slowly rotating low-gravity tank Theory

The equilibrium configuration of a bubble in a rotating liquid confined by flat axial boundaries (baffles) is found. The maximum baffle spacing assuring bubble confinement is bounded from above by the natural length of a bubble in an infinite medium under the same conditions. Effects of nonzero contact angle are minimal. The problem of dynamic stability is posed. It can be solved in the limit of rapid rotation, for which the bubble is a long cylinder. Instability is to axisymmetric perturbations; nonaxisymmetric perturbations are stable. The stability criterion agrees with earlier results.

Gans, R. F.↗

On the Interfacial Assembly of Anisotropic Amphiphilic Janus Particles

It has been shown both theoretically and experimentally that amphiphilic Janus particles are the most effective solid surfactants to stabilize interfaces. In most cases, the Janus particles investigated have uniform morphologies with Janus boundaries dividing the particle into halves. However, there are many examples of Janus particles where the hydrophilic and hydrophobic domains are not equally distributed. The effects of this uneven domain distribution on the mechanism and kinetics of Janus particle assembly, and final equilibrium state are not well-understood. Dynamic pendant drop tensiometry offers a means to probe both the equilibrium assembly and the kinetics and mechanism of assembly. Here, in this work, the interfacial kinetics and assembly of spherical anisotropic Janus particles are investigated using dynamic pendant drop tensiometry. Systematic studies quantifying the time-dependent interfacial behavior as a function of Janus particle morphology, chemical composition, particle concentration, and NaOH and HCl concentration are performed. These studies shed light on the assembly mechanism of more complex Janus particle morphologies and highlight their effectiveness as interface stabilizers.

36 MATERIALS SCIENCE↗

Dynamic Interfacial Architectures: Cruciferin‐Stabilized Oil/Water Interfaces for Sustainable Emulsions

Stabilizing oil-water interfaces in emulsions by plant-based proteins provides sustainable and tunable ways for designing emulsions with specific properties, for food, healthcare, and pharmaceuticals. Cruciferin, a protein from rapeseed, has great potential as green emulsifier, but details about its structure and mobility at oil-water interfaces are largely unknown. Here, these properties are studied with small angle neutron and x-ray scattering, and neutron spin echo spectroscopy, analyzed by atomistic modelling of scattering curves and coarse-grained modelling, to gain insight into interface coverage, and molecular conformation and mobility at the interface. Cruciferin assumes trimeric conformations at the interface, as in solution, but with its protrusions from the central core of the subunits (“arms”) more compressed. Interfacial mobility is only marginally lower than in solution, indicating the arms still transiently extend and preserve a network, for the first time revealing the mechanism how cruciferin forms highly elastic 2d gel-like oil-water interfaces, as observed in macroscopic rheology. The high interfacial mobility may help in self-repairing non-stabilized interfacial fractions, reducing coalescence. These findings provide a deeper molecular level understanding of proteins at oil-water interfaces, which can stimulate development of new plant-based emulsion products, and contribute to the global protein transition.

cruciferin↗

EVA-glass interface bond stability

The ethylene vinyl acetate/glass interface bond stability was investigated. Special methods to determine the structure of polymer/glass interface were developed. Structural changes related to hydrothermal degradation of polymer/glass interface are examined. Methods to inhibit the degradation reaction which occur at polymer/glass interface are developed.

Koenig, J. L.↗

Computation-guided discovery of coating materials to stabilize the interface between lithium garnet solid electrolyte and high-energy cathodes for all-solid-state lithium batteries

All-solid-state batteries with a lithium metal anode, enabled by lithium garnet solid electrolytes such as Li 7 La 3 Zr 2 O 12 (LLZO), are a promising next-generation energy-storage technology. The further development of all-solid-state battery requires the integration of high-energy cathodes such as LiNi 1-x-y Mn x Co y O 2 (NMC) with the garnet solid electrolyte with stable and low-resistance interfaces, which requires a coating layer to stabilize the interface during high-temperature sintering and electrochemical cycling. In order to guide the future development of interfacial coatings, we perform high-throughput thermodynamic analyses based on first-principles computation to investigate the stability of LLZO garnet and high-energy NMC cathodes with a wide range of materials chemistries. Here our study reveals the factors governing the materials stability with LLZO garnet and NMC cathodes, and identifies the mechanisms of good coating layers stable with LLZO and NMC. In addition to classifying known coating layers, our study provides detailed guiding charts and multiple new materials systems as promising coatings for stabilizing LLZO—NMC interfaces to enable high-energy-density garnet-based all-solid-state batteries. Our demonstrated computation scheme and high-throughput analyses are generally applicable to investigate and screen coating materials for stabilizing interfaces in energy-related applications.

25 ENERGY STORAGE↗

Effects of Anion Clusters at Solid-State Electrolyte and Electrode Interfaces

Stability and transport properties at the electrolyte-electrode interface are of great importance to the performance of all-solid-state batteries with solid-state electrolytes (SSEs). Most recent studies have shown that mono-/poly-anion clusters that are either original contained or doped in the SSE can lead to intriguing (transport, electronic, and mechanical) properties [1-6]. However, the effects of anion clusters on the SSE-electrode interfaces are unknown. Here, we will investigate such effects and unravel the working mechanisms using phase/reactivity analysis and explicit interface modeling.

Fang, Hong↗

Dynamic stability of a crude oil/brine interface: Effect of anion type

The chemical composition of the aqueous phase plays an essential role in water-based enhanced-oil recovery processes. The aqueous phase ionic profile affects the snap-off response of a crude oil-brine system by linking it to the brine-crude oil interfacial rheology. In this work, we focus on the effect of the anion on the snap-off response. To this end, a sample of crude oil from the Minnelusa Sandstone formation in Wyoming was selected, and several aqueous solutions were prepared with salts containing sodium cation and different anions (chlorides, sulfates, and phosphates) at two ionic strength values, 0.6 M and 6 mM, as cases of high- and low-salinity water. Interfacial tension, interfacial viscoelasticity and interface stability were analyzed as functions of aging time using pendant drop, dilatational rheology, and liquid bridge techniques, respectively. Here the results show that solutions with higher ionic strength led to the formation of more rigid interfaces, i.e. higher elastic modulus, and faster formation kinetics. In the low-salinity regime, solutions with polyvalent anions produce more viscoelastic interfaces at faster rates than solutions with monovalent anions. Finally, an excellent correlation (R 2 greater than 0.97) between the relative stability of the interfacial film, predicted in liquid bridge tests, and the ratio of interfacial tension and interfacial elastic modulus was found.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stability of interfaces with mesh refinement

A study is conducted of the stability of mesh refinement in space and time for several different interface equations and finite-difference approximations. First, a root condition which implies stability for the initial-boundary value problem for this type of interface is derived. From the root condition, the stability of several interface equations is proved, using the maximum principle. In some cases, the final verification steps can be done analytically; in other cases, a simple computer program has been written to check the condition for values of a parameter along the boundary of the unit circle. Using this method, stability for Lax-Wendroff with all the interface conditions considered, and for Leapfrog with interpolation interface conditions when the fine and coarse grids overlap is proved.

Berger, M. J.↗

Coupled Growth in Hypermonotectics

The overall objective of this project is to obtain a fundamental understanding of the physics controlling solidification processes in immiscible alloy systems. The investigation involves both experimentation and the development of a model describing solidification in monotectic systems. The experimental segment was designed to first demonstrate that it is possible to obtain interface stability and steady state coupled growth in hypermonotectic alloys through microgravity processing. Microgravity results obtained to date have verified this possibility. Future flights will permit experimental determination of the limits of interface stability and the influence of alloy composition and growth rate on microstructure. The objectives of the modeling segment of the investigation include prediction of the limits of interface stability, modeling of convective flow due to residual acceleration, and the influence of surface tension driven flows at the solidification interface. The study of solidification processes in immiscible alloy systems is hindered by the inherent convective flow that occurs on Earth and by the possibility of sedimentation of the higher density immiscible liquid phase. It has been shown that processing using a high thermal gradient and a low growth rate can lead to a stable macroscopically planar growth front even in hypermonotectic alloys. Processing under these growth conditions can avoid constitutional supercooling and prevent the formation of the minor immiscible liquid phase in advance of the solidification front. However, the solute depleted boundary layer that forms in advance of the solidification front is almost always less dense than the liquid away from the solidification front. As a result, convective instability is expected. Ground based testing has indicated that convection is a major problem in these alloy systems and leads to gross compositional variations along the sample and difficulties maintaining interface stability. Sustained low gravity processing conditions are necessary in order to minimize these problems and obtain solidification conditions which approach steady state.

Andrews, J. Barry↗

Mesoscale Polymer Surfactants: Photolithographic Production and Localization at Droplet Interfaces

Stabilization of fluid droplets, classically as oil-in-water or water-in-oil emulsions, is typically conducted using molecular surfactants or small particulates that localize at oil-water interfaces. In this paper, we describe a method whereby thin polymer films are converted photolithographically to ribbon-like mesoscale objects, which in turn adsorb to fluid inter-faces where they extend as appendages, or arms, from the droplet surface. These “mesoscale polymer surfactants”, or MPSs, were prepared from thin polymer films containing reactive functional moieties, including coumarin for photo-crosslinking, triphenylsulfonium for photoacid generation, and tert-butyl ester for solubility switching. The resultant MPSs, prepared initially on Si substrates, were released into water to reveal an exquisite shape sensitivity (forming straight, bent, or helical structures) and affinity for droplet interfaces based on their preparation conditions and the properties of the surrounding liquid. Notably, the lithographic techniques employed were amenable to differentiating the wettability of MPS segments, affording access to diblock-like MPSs which adhered to dispersed droplets via their hydrophobic segments, allowing their hydrophilic segments to extend into the continuous phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of flow on interface shape stability in low gravity

The objectives are to: (1) Understand the influence in low gravity of flow on interface shape. For example, document and control the influence of axial flow on the Plateau-Rayleigh instability of a liquid bridge; and (2) Extend the ground-based density-matching technique of low gravity simulation to situations with flow; that is, develop Plateau chamber experiments for which flow can be controlled. Containerless containment of liquid by surface tension has broad importance in low gravity. For space vehicles, the behavior of liquid/gas interfaces is crucial to successful liquid management systems. In microgravity science, free interfaces are exploited in various applications. Examples include float-zone crystal growth, phase separation near the critical point of liquid mixtures (spinoidal decomposition) and quenching of miscibility gap molten metal alloys. In some cases, it is desired to stabilize the capillary instability while in others it is desired to induce capillary breakup. In all cases, understanding the stability of interface shape in the presence of liquid motion is central.

Steen, Paul H.↗

Ion transport through reconfigurable nanoparticle-surfactant stabilized droplet interface bilayers

Despite their adaptability and mechanical stability, Pickering emulsions based on the interfacial assembly of colloidal particles have not found use in iontronics, since the dense interfacial packing of micron-sized particles precludes functional connectivity between two droplets. In this work, we introduce a chemically reconfigurable droplet interface bilayer (DIB) platform based on the interfacial assembly of nanoparticle-surfactants (NPSs) that enables spontaneous or field-induced formation of ion-conducting nanochannels, eliminating the need of ionophores or nanochannel-forming proteins. These nanoscopic channels emerge from packing defects in the jammed interfacial assemblies of the charged NPSs and support size and charge selective, hysteretic ion transport governed by interfacial electrostatics and dimensional constraints. The NPS-DIBs show short-term and long-term plasticity, hallmarks of neuromorphic behavior, that are mediated by the structural and chemical design of the bilayer. These assemblies establish a versatile, chemically tunable platform that couples soft-matter mechanics with interfacial ionic functionality, offering a robust foundation for soft iontronic systems.

36 MATERIALS SCIENCE↗

Unveiling the Role of Lithium Iodide in Stabilizing Solid Interfaces in All-Solid-State Li Metal Batteries

A critical challenge in all-solid-state lithium metal batteries (ASSLMBs) is achieving a stable interface between the lithium metal anode and the solid electrolyte. Leveraging its success in Li/I 2 batteries, lithium iodide has garnered significant attentions for its potential to enhance interfacial stability and overall cell performance in ASSLMBs. Here, we elucidate the role of lithium iodide in stabilizing the solid interface in all-solid-state Li metal batteries with a Li argyrodite electrolyte, particularly focusing on its influence on lithium deposition behavior and interfacial evolution. Through in situ optical imaging, we demonstrate more uniform lithium deposition on an iodide-contained argyrodite electrolyte compared to a chloride-based counterpart. Complementary density functional theory calculations attribute improved lithium plating behavior to the enhanced lithiophilicity and better ionic conductivity of lithium iodide at the solid interface, effectively reducing localized current density. In conclusion, these findings provide useful insights into the mechanisms through which lithium iodide enhances the interfacial stability in ASSLMBs.

Anions↗

Complexions at the iron-magnetite interface

Synthesizing distinct phases and controlling crystalline defects are key concepts in materials design. These approaches are often decoupled, with the former grounded in equilibrium thermodynamics and the latter in nonequilibrium kinetics. By unifying them through defect phase diagrams, we can apply phase equilibrium models to thermodynamically evaluate defects—including dislocations, grain boundaries, and phase boundaries—establishing a theoretical framework linking material imperfections to properties. Using scanning transmission electron microscopy (STEM) with differential phase contrast (DPC) imaging, we achieve the simultaneous imaging of heavy Fe and light O atoms, precisely mapping the atomic structure and chemical composition at the iron-magnetite (Fe/Fe 3 O 4 ) interface. We identify a well-ordered two-layer interface-stabilized phase state (referred to as complexion) at the Fe[001]/Fe 3 O 4 [001] interface. Using density-functional theory (DFT), we explain the observed complexion and map out various interface-stabilized phases as a function of the O chemical potential. The formation of complexions increases interface adhesion by 20% and alters charge transfer between adjacent materials, impacting transport properties. Our findings highlight the potential of tunable defect-stabilized phase states as a degree of freedom in materials design, enabling optimized corrosion protection, catalysis, and redox-driven phase transitions, with applications in materials sustainability, efficient energy conversion, and green steel production.

36 MATERIALS SCIENCE↗