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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Understanding interfacial crystallization dynamics on carbon fiber reinforced polypropylene composite manufacturing

Reinforcing polymers with discontinuous fibers improves mechanical properties, such as strength and stiffness, and in some cases achieve isotropic properties, rendering them suitable for various engineering applications. Matrix materials are generally highly engineered thermosets (e.g. crosslinked epoxies), bonded to the fiber periphery by proprietary surface and sizing chemistries. Semicrystalline thermoplastic matrices are less utilized due to poor fiber-matrix bonding resulting in inefficient interfacial load-transfer in reinforced composites. However, flexibility with melt-processing or molding conditions can be leveraged to promote non-covalent interfacial bonding between matrix and fiber via crystallization of the matrix onto fiber surface. In the present study, we utilize a co-mingle chopped carbon and isotactic polypropylene fibers to form isotropic composites, tailoring interfacial immobilized matrix or interphase morphology to optimize performance through precise control of thermal processing/molding windows. Calorimetry and optical microscopy were employed to investigate the impact of carbon fiber at various volume fractions (10, 20, and 30 %) on isotactic polypropylene crystallization and mechanical performance. Variations in mechanical properties correspond to the structural evolution of the interfacial region and are correlated to underlying microstructural attributes using wide-angle X-ray scattering, thermal analysis, and low-field nuclear magnetic resonance spectroscopy. These results provide a practical framework for the manufacturing of thermoplastic matrix composites. In conclusion, the results presented provide a guide for the strategic optimization of interphase design, showcasing tailorable tensile strengths which outperform any isotactic polypropylene carbon fiber composites previously reported in literature.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Interface engineering of colloidal CdSe quantum dots thin films as acid-stable photocathodes for solar-driven hydrogen evolution

Colloidal semiconductor quantum dots-based (CQD) photocathodes for solar-driven hydrogen evolution have attracted significant attention due to their tunable size, nanostructured morphology, crystalline orientation, and band-gap. Here, we report a thin film heterojunction photocathode composed of organic PEDOT:PSS as a hole transport layer, CdSe CQDs as a semiconductor light absorber, and conformal Pt layer deposited by atomic layer deposition (ALD) serving as both a passivation layer and cocatalyst for hydrogen evolution. In neutral aqueous solution, a PEDOT:PSS/CdSe/Pt heterogeneous photocathode with 200 cycles of ALD Pt produces a photocurrent density of -1.08 mA/cm 2 (AM1.5G, 100 mW/cm 2 ) at a potential of 0 V vs. RHE (j 0 ) in neutral aqueous solution, which is nearly 12 times that of the pristine CdSe photocathode. This composite photocathode shows an onset potential for water reduction at +0.46 V vs. RHE and long-term stability with negligible degradation. In acidic electrolyte (pH = 1), where the hydrogen evolution reaction is more favorable but stability is limited due to photocorrosion, a thicker Pt film (300 cycles) is shown to greatly improve the device stability and a j 0 of -2.14 mA/cm 2 is obtained with only 8.3% activity degradation after 6 h, compared to 80% degradation under the same conditions when the less conformal electrodeposition method is used to deposit the Pt layer. Electrochemical impedance spectroscopy and time-resolved photoluminescence results indicate that these enhancements stem from a lower bulk charge recombination rate, higher interfacial charge transfer rate, and faster reaction kinetics. In conclusion, we believe that these interface engineering strategies can be extended to other colloidal semiconductors to construct more efficient and stable heterogeneous photoelectrodes for solar fuel production.

42 ENGINEERING↗
DOE OSTI2023

Engineering bimetallic interfaces and revealing the mechanism for carbon dioxide electroreduction to C 3+ liquid chemicals

Reduction reaction of CO 2 (CO 2 RR) to liquid C 3+ chemicals is a net-zero-carbon process and can increase local resiliency to power outages and fuel consumption. The mechanism and the catalyst design rules of CO 2 RR-to-C 3+ are unknown. Engineering bimetallic interface (e.g., Pd/Au) to tune the intermediate adsorption is promising for promoting C 3+ formation. Our density functional theory (DFT) calculations find that *CH 2 could be the key intermediate and C 1 -CH 2 coupling could be the rate-limiting step to generate C 3+ . High CO surface coverages can promote the bimetallic interfacial sites, lower the energetics of the C 1 -CH 2 coupling step, and enhance the C 3+ formation. We further construct a volcano plot of C 1 -CH 2 kinetics as a function of the binding strength of key intermediate *CH 2 via engineering the d-band center of the interfacial site. Our findings could guide the rational design of bimetallic interfaces and their near-surface microenvironment for enhancing CO 2 RR-to-C 3+ .

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

Structural Implications of Interfacial Hydrogen Bonding in Hydrated Wyoming-Montmorillonite Clay

Montmorillonite (MMT) clay - a layered porous nanomaterial used as seals in engineered waste containment barriers for spent nuclear fuel - adopts discrete hydration/swelling states depending upon surrounding water and ion activities and confining pressure. The structure of nanoconfined water and charge-balancing counterions in the clay mineral interlayers dictate the swelling and mechanical behavior of MMT, so a molecular model for this clay with high structural fidelity is required to accurately predict the reliability of long-term nuclear waste storage. Here, we present a molecular model for MMT that is based on high resolution transmission electron microscopy of Wyoming-MMT single crystals. Imaging data unambiguously show a cis-vacant arrangement of structural hydroxyl groups in the octahedral sheet, whereas existing molecular models assume a centrosymmetric trans-vacant configuration for MMT. Furthermore, using atomistic simulations, we find that the cis-vacant arrangement of structural hydroxyl groups significantly affects the structure of adsorbed water yielding a larger population of hydrogen bonds with bridging oxygens on the tetrahedral sheet and weak hydrogen bonding between the hydroxyl groups in the octahedral sheet and water in the clay mineral interlayers. As a result, water adsorbed in the interlayer is more "ice-like", with stronger ordering and lower density, although the diffusivity of the interlayer species is not significantly diminished. Our improved structural model for MMT provides insight into the energetics of water adsorption, which ultimately dictates its pore- to macro-scale swelling, transport, and fracture properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Engineered Thin Diffusion Layers for Anion-Exchange Membrane Electrolyzer Cells with Outstanding Performance

Anion-exchange membrane electrolyzer cells (AEMECs) are one of the most promising technologies for carbon-neutral hydrogen production. Over the past few years, the performance and durability of AEMECs have substantially improved. Herein, we report an engineered liquid/gas diffusion layer (LGDL) with tunable pore morphologies that enables the high performance of AEMECs. The comparison with a commercial titanium foam in the electrolyzer indicated that the engineered LGDL with thin-flat and straight-pore structures significantly improved the interfacial contacts, mass transport, and activation of more reaction sites, leading to outstanding performance. We obtained a current density of 2.0 A/cm 2 at 1.80 V with an efficiency of up to 81.9% at 60 °C under 0.1 M NaOH-fed conditions. The as-achieved high performance in this study provides insight to design advanced LGDLs for the production of low-cost and high-efficiency AEMECs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Water Migration and Swelling in Engineered Barrier Materials for Radioactive Waste Disposal

Deep, underground repositories are needed to isolate radioactive waste from the biosphere. Because bentonite is an integral component of many multibarrier repository systems, information on the hydraulic behavior of bentonite is crucial for modeling the long-term viability of such systems. In this paper the hydraulic behavior of bentonite samples was analyzed as a function of aggregate size, and samples were subjected to hydrothermal treatments involving contact with NaCl, KCl, and deionized water. Neutron and X-ray imaging were used to quantify water sorption into packed bentonite samples and bentonite swelling into the water column. The distance between the original clay-water interface and the wetting front was determined as a function of time. Average water uptake exhibited a square-root-of-time dependence in freshly prepared samples, but more variable rates were observed for samples previously in contact with water. The radiography was supported by small-angle neutron scattering analysis and ultra-small-angle neutron scattering analysis of aggregate size distributions and by inelastic neutron scattering to understand the physicochemical environment of the sorbed water. Results showed that hydrothermal treatment with KCl had the greatest effect of increased water transport in the bentonite, possibly as a result of the interaction of K + with smectite layers in the clay.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Chemo–mechanical properties of carbon fiber reinforced geopolymer interphase

Geopolymers, as a potentially environmentally friendly alternative to Portland cement, are increasingly attracting attention in the construction industry. Various methods have been applied for customizing the properties of geopolymers and improving their commercial viability. One of the promising methods for refining the properties of geopolymers such as their toughness is the use of short fibers. The effectiveness of a high-strength short fiber in the geopolymer matrix is largely dependent on the interfacial bonding between the fiber and its surrounding matrix. While the importance of this interfacial chemistry is highlighted in the literature, the characteristics of this bonding structure have not been fully understood. In this paper, we aim to investigate the bonding mechanism between the carbon fiber and metakaolin-based geopolymer matrix. For the first time, the existence and nature of the chemical bonding at the interfacial region (interphase) between carbon fiber and geopolymer matrix has been revealed. X-ray pair distribution function computed tomography (PDF-CT), field emission-scanning electron microscopy imaging, and nanoindentation techniques are employed to discern the chemo-mechanical properties of the interphase. PDF-CT results show the emergence of a new atom-atom correlation at the interfacial region (around 1.82 angstrom). This correlation is a characteristic of interfacial bonding between the fiber and its surrounding matrix, where the existence of chemical linkages (potentially Al-V-O-C) between fibers and the matrix contributes to the adhesion between the two constituents making up the composite. Due to such chemical bonding, the nanomechanical properties of the interfacial region fall between that of the carbon fiber and geopolymer. The combination of advanced techniques is proved useful for enhancing our understanding of the interfacial chemistry between fibers and the binding matrix. This level of knowledge facilitates the engineering of composite systems through the manipulation of their nanostructure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Doping Metallic Grain Boundaries to Control Atomic Structure and Damage Tolerance (Final Report)

The interfaces between crystals, known as grain boundaries, often act as sites for crack and void nucleation during plastic deformation of metallic materials. While it is known that interfacial character and structural state can greatly influence this damage nucleation process, the current level of control over such details is extremely limited. The objective of this project was to obtain a fundamental understanding of how metallic grain boundary structure can be controlled through intelligent doping, with the idea of inducing planned grain boundary phases or complexions. The effect of complexion structure on dislocation accommodation mechanisms was studied, to improve the field’s understanding of damage nucleation at interfaces. While mechanical damage was the primary focus, the project showed that amorphous complexions can also improve a material’s resistance to radiation damage, providing a single materials design concept that can address multiple important technological areas. This research used a combination of computational, experimental, and characterization techniques to isolate and understand the importance of nanoscale grain boundary structure and interfacial chemistry. The fundamental insights provided by this project enable the creation of advanced engineering metals with improved damage tolerance.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Mixed matrix membranes for post-combustion carbon capture: From materials design to membrane engineering

Mixed matrix materials (MMMs) containing nanofillers dispersed in continuous polymer matrices have emerged as an exciting and versatile platform to develop membranes with superior CO 2 /N 2 separation performance for post-combustion carbon capture. Both polymers and nanofillers can be vertically designed and engineered to combine the advantages of excellent processability (derived from polymers) and strong size-sieving ability or/and significant permanent porosity (originated from nanofillers). However, the MMMs face major challenges, such as interfacial incompatibility, particle agglomeration, and poor thin-film formability. This report provides a comprehensive yet critical review of various polymers and nanofillers (such as metal-organic frameworks, covalent organic frameworks, and two-dimensional materials) with promising CO 2 /N 2 separation properties. We exhaustively describe strategies to improve interfacial compatibility, such as in situ syntheses of polymers and nanofillers and functionalization of both components to improve adhesion. Moreover, we highlight various approaches to engineer the MMMs into thin-film composite (TFC) membranes. The review reveals the structure/property relationship in these MMMs and outlines the challenges and opportunities to realize their potential for practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Surface engineering to enhance heat generation and joint strength in dissimilar materials AZ31 and DP590 ultrasonic welding

A multiscale simulation approach was developed and employed to optimize the sheet surface conditions for higher interfacial temperature and joint strength in ultrasonic welding of magnesium alloy AZ31 and dual-phase steel DP590. First, a mesoscale model was used to study the relationship between friction coefficient and surface roughness, which can be modified by various engineering methods. Then a macroscopic process model was employed to study the effects of surface roughness on heat generation, indicating that a temperature increase can be achieved with rougher surfaces on two sides of both DP590 and AZ31 sheets. Samples prepared by sanding and filing, as well as grinding, were first characterized for surface roughness and then welded under ultrasonic vibration. An infrared camera was used to measure temperatures in situ for model validation. Overall, lap shear test results for the welded joint showed that the joint strength can be improved by 10~25% using filing and round grinding methods as a result of the enhanced heat generation and mechanical interlocking on the interface.

42 ENGINEERING↗
DOE OSTI2022

A mechanism for reduced compression in indirectly driven layered capsule implosions

High-yield implosions on the National Ignition Facility rely on maintaining low entropy in the deuterium–tritium fuel, quantified by its adiabat, in order to efficiently couple energy to the hot spot through high compression of the fuel layer. We present very-high-resolution xRAGE simulation results that study the impacts of interfacial mixing and the jetting of materials due to surface defects, defects on internal interfaces, voids, and engineering features on fuel layer compression. Defects and voids are typically neglected in implosion simulations due to their small size and three-dimensional geometry. Our results showed that supersonic jets of material arise through weak spots in the shell at peak implosion velocity that prevent uniform compression of the fuel layer even when they do not introduce contaminant into the hot spot. This occurs despite maintaining low fuel entropy, since the formation of the weak spots involves nonradial displacement of fuel mass. In contrast, simulations show that fuel–ablator mixing due to interfacial instabilities has a much smaller impact on compression. We show that defects on interior interfaces of plastic capsules decrease compression by 15% to 25% and interfacial mixing between the ablator and fuel decreases compression by less than 1% for implosions with plastic or high-density carbon (HDC) ablators. For low adiabat implosions, the impact of jetting seeded by the support tent can also decrease the compression by 25%. We demonstrate that the inclusion of interior defects in simulations can explain the inferred compression in two fielded plastic capsule implosions and that the inclusion of voids, for which available characterization has large uncertainties, in simulations of HDC capsule implosions has a qualitatively consistent impact. This mechanism offers a potential explanation for persistently overestimated fuel compression in design simulations of layered implosions on the National Ignition Facility.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2018

Interfacial and Transport Property Measurements of Liquid Sodium within a Porous Structure

The sodium thermal electrochemical converter (Na-TEC) is a heat engine that generates electricity via the isothermal expansion of sodium ions through a beta”-alumina solid-electrolyte. The transfer of liquid sodium from a low-pressure condenser to a high-pressure evaporator is necessary to complete the thermodynamic cycle for this conversion process. A unique sodium capillary pump for the Na-TEC is proposed, whereby low-pressure sodium vapor is condensed within a non-wetting (i.e. contact angle > π/2) porous sample. The curvature created at this non-wetting condensation interface supplies a directed force upon the liquid sodium that effectively “pushes” it towards a high pressure region, rather than a traditional capillary wick that “pulls” the liquid. Porous structures made of stainless steel 316 are commercially available, and this material is non-wetting to sodium at the relevant temperature range of the Na-TEC condenser (500K – 673K). An experimental set-up is used to measure several interfacial and transport properties of the condensed sodium within this porous structure. These properties include the temperature dependent Laplace pressure generated at the phase change interface and the permeability of the porous structure. For the former, liquid sodium is in contact with the porous structure and is progressively pressurized with argon gas in increments of ~ 5 kPa until the sodium “breaks through” and the liquid begins to flow. This breakthrough pressure is determined when electrical contact is established between the flowing liquid metal and a set of electrodes cemented into the flow path. The velocity of the flowing sodium can also be measured with these electrodes, and the permeability is then determined by fitting velocity data to the classical Darcy law. Statistically significant results of these measurements, taken at multiple sodium temperatures, are presented. Furthermore, contact angle measurements of sessile sodium drops on stainless steel 316 are demonstrated. This contact angle information is used to define an effective pore radius for the porous structure, which is then validated with microscopy. All the physical parameters described herein are used as inputs in a condensation model to predict the mass flowrate of condensing sodium under a given pressure gradient across the porous structure. This condensation model is used to design the capillary pump for the Na-TEC.

14 SOLAR ENERGY↗
DOE OSTI2026

Final Technical Report for DE-SC0021049: Manipulating interfacial reactivity with atomically layered heterostructures

This final technical report summarizes the work accomplished in this DOE Early Career Research Program project that has established moiré superlattice materials and two-dimensional (2D) heterostructures as a highly tunable platform for controlling heterogeneous charge transfer (ET) kinetics at solid-liquid interfaces. By precisely engineering van der Waals heterostructures of atomically thin 2D materials, particularly bilayer and trilayer graphene with controlled twist angles, this project demonstrated systematic control of interfacial charge transfer rates spanning three orders of magnitude. This research addresses fundamental questions about how electronic structure, charge localization, and atomic layer-dependent properties govern charge transfer at electrochemical interfaces, with broad implications for energy conversion, electrocatalysis, and next-generation electrochemical devices.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Distribution of nickel(II) ions adsorbed at the muscovite mica (001)-water interface determined by in-situ resonant anomalous X-ray reflectivity

Mineral-water interfaces mediate adsorption, ion exchange, and secondary mineral formation that control element mobility in natural and engineered systems. Reliable prediction and control of these processes require a fundamental understanding of the interfacial structure that links adsorbed ion speciation to macroscopic sorption capacity and strength. Here, we determine atomic-scale changes in hydration and distribution of Ni(II) at the muscovite mica (001)-water interface using in situ high-resolution X-ray reflectivity (XR) and resonant anomalous X-ray reflectivity (RAXR) at 1 mM NiCl2 and pH 5.7. XR reveals reorganization of the primary hydration structure relative to that in deionized water: the water layer adsorbed in the cavity sites at a height of ~1.3 Å disappears, while distinct solution layers emerge at ~2.3, ~4.1, and ~5.6 Å above the basal oxygen plane. RAXR resolves three interfacial Ni(II) species: a dominant outer-sphere complex at 3.65 Å (~80% of the total coverage), a minor inner-sphere complex at 0.75 Å, and a low-coverage, more distant outer-sphere species at 5.63 Å. These three adsorbed Ni(II) species account for a total Ni(II) coverage of 0.54 ± 0.02 ion per unit cell area that compensates for the surface charge. These results highlight the role of interfacial hydration in controlling the speciation and stability of adsorbate cations on the negatively charged mica surface, providing quantitative insight into predicting the geochemical behavior of divalent metal cations in the aqueous environments.

Lee, Sang Soo↗
DOE OSTI2022

Nitrile-Containing Renewable Polymers Based on Lignin, (CRADA) No. NFE 1807437 (CRADA Final Report)

Lignin remains one of the world’s largest sources of renewable carbon, with significant potential to positively impact our carbon footprint by replacing fossil-fuel derived materials, including engineering thermoplastics and their composites. Efforts to incorporate significant quantity of lignin into engineering thermoplastics as anything other than an inert filler have to date been largely unsuccessful, however due to limitations imposed by the degradation temperature of the lignin (220 °C) and poor compatibility between the lignin and non-polar or slightly polar polymers. Recent work at Oak Ridge National Laboratory has however shown under the right conditions excellent compatibility between lignin and nitrile containing rubber compounds such as nitrile-butadiene rubber (NBR). The present work extends these findings to the incorporation of lignin into acrylonitrile-butadiene-styrene (ABS) engineering plastics. While simple binary mixing of lignin into commercial ABS resins leads to poor interfacial adhesion and resultant low toughness and ductility, appropriate matching of the lignin and ABS components, and as appropriate compatibilizing agents, leads to polymer blends incorporating 20-35% by weight lignin with a useful range of mechanical properties for many current ABS applications. By modifying the composition, the balance of properties can be readily tailored to meet the demands of specific end-user applications.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Atomic- and Molecular-Scale Interphase Engineering for High-Performance Solid-State Batteries

Solid-state batteries (SSBs) promise a decisive advance beyond conventional Li-ion systems, yet their development remains constrained by persistent solid–solid interfacial instabilities that degrade performance and durability. Interfaces between solid electrolytes and both cathodes and Li metal often exhibit poor wettability, limited physical contact, and high charge–transfer resistance, leading to chemical decomposition, mechanical failure, and impedance growth. Overcoming these limitations requires interphase engineering with atomic-scale precision—capabilities that conventional coating methods cannot reliably deliver. Atomic layer deposition (ALD) and molecular layer deposition (MLD) uniquely meet this need by enabling ultrathin, conformal, and composition-tunable films that stabilize reactive surfaces, suppress parasitic reactions, and regulate Li-metal morphology. Importantly, this Perspective highlights ALD/MLD systems that have already demonstrated effectiveness in liquid-electrolyte cells and discusses how these validated strategies can be deliberately translated to solid-state architectures. By grounding future directions in experimentally proven concepts rather than speculative hypotheses, we outline how atomic- and molecular-scale design principles can accelerate the development of robust, high-performance SSB technologies.

atomic and molecular layer deposition↗
DOE OSTI2021

Interface Aspects in All‐Solid‐State Li‐Based Batteries Reviewed

Abstract Extensive efforts have been made to improve the Li‐ionic conductivity of solid electrolytes (SE) for developing promising all‐solid‐state Li‐based batteries (ASSB). Recent studies suggest that minimizing the existing interface problems is even more important than maximizing the conductivity of SE. Interfaces are essential in ASSB, and their properties significantly influence the battery performance. Interface problems, arising from both physical and (electro)chemical material properties, can significantly inhibit the transport of electrons and Li‐ions in ASSB. Consequently, interface problems may result in interlayer formation, high impedances, immobilization of moveable Li‐ions, loss of active host sites available to accommodate Li‐ions, and Li‐dendrite formation, all causing significant storage capacity losses and ultimately battery failures. The characteristic differences of interfaces between liquid‐ and solid‐type Li‐based batteries are presented here. Interface types, interlayer origin, physical and chemical structures, properties, time evolution, complex interrelations between various factors, and promising interfacial tailoring approaches are reviewed. Furthermore, recent advances in the interface‐sensitive or depth‐resolved analytical tools that can provide mechanistic insights into the interlayer formation and strategies to tailor the interlayer formation, composition, and properties are discussed.

25 ENERGY STORAGE↗
DOE OSTI2026

An Organic Carboxylate Host for Stable Sodium Metal Batteries

Sodium metal batteries (SMBs) hold great promise for the development of high-energy, sustainable energy storage solutions, but their practical deployment is hampered by unstable solid electrolyte interphases, uncontrollable sodium dendrite growth, and low Coulombic efficiency (CE) during repeated Na plating/stripping cycles. To address these challenges, we introduce an organic interlayer, containing perylenetetracarboxylic dianhydride sodium salt (Na4PT), on the surface of Cu current collector. This interlayer forms a sodiophilic organic interphase that lowers the nucleation barriers for sodium deposition and guides the formation of the interphase through polar carbonyl/carboxylate sites and a π-conjugated organic framework. A dendrite-free sodium metal anode is achieved using Na4PT coated Cu current collector. Under capacity-limited Na plating/stripping, Na||Na4PT@Cu half-cells deliver reversible capacities of 500 and 1,000 mAh g−1 at 0.1 and 1 A g−1 for 500 cycles with average CE above 99%. Post-cycling scanning electron microscopy and X-ray photoelectron spectroscopy measurements confirm that Na4PT@Cu promotes compact and uniform Na deposits and supports the formation of a stable interphase with reduced parasitic decomposition, directly correlating interfacial chemistry/morphology with high plating/stripping reversibility. These results highlight organic carboxylate coating as a practical interface engineering strategy for dendrite-free SMBs.

Chen, Chengxiang [University of Miami]↗