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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.

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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Evidence for Interfacial Octahedral Coupling as a Route to Enhance Magnetoresistance in Perovskite Oxide Superlattices

Engineering octahedral rotations in oxide heterostructures is a promising route for controlling magnetic properties in perovskites, with recent work focusing on magnetic-ordering temperatures and magnetic anisotropies. Here the effects of interfacial octahedral coupling on magnetoresistance are demonstrated in a series of (La 0.7 Sr 0.3 MnO 3 ) n /(LaFeO 3 ) 10 superlattices grown on (001)- and (111)-oriented SrTiO 3 substrates. The different crystallographic orientations allow for the interfacial octahedral connectivity to be tuned, with weaker interfacial coupling present at the (001)-oriented than the (111)-oriented structures as revealed by density functional theory calculations. In n = 14 superlattices, the effect of orientation on the physical properties is minimal with both (001)- and (111)-oriented samples exhibiting similar magnetoresistance. As the fraction of interfacial volume within the LSMO layers is increased by decreasing n, the magnetoresistive behavior of the samples diverges with significantly larger magnetoresistance magnitudes present in the (111)-oriented superlattices. Furthermore, the results are consistent with octahedral coupling playing a greater role in the functional properties at (111)-heterointerfaces and demonstrate a structure-driven approach to tuning interfacial magnetoresistance in complex-oxide heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Bipolar membrane polarization behavior with systematically varied interfacial areas in the junction region

The palette of applications for bipolar membranes (BPMs) has expanded recently beyond electrodialysis as they are now being considered for fuel cell and electrolysis applications. Their deployment in emerging electrochemical technologies arises from the need to have a membrane separator that provides disparate pH environments and to prevent species crossover. Most materials research for BPMs has focused on water dissociation catalysts and less emphasis has been given to the design of the polycation–polyanion interface for improving BPM performance. Here, soft lithography fabricated a series of micropatterned BPMs with precise control over the interfacial area in the bipolar junction. Polarization experiments showed that a 2.28× increase in interfacial area led to a 250 mV reduction in the onset potential. Additionally, the same increase in interfacial area yielded marginal improvements in current density due to the junction region being under kinetics-diffusion control. A simple physics model based on the electric field of the junction region rationalized the reduction in the overpotential for water dissociation as a function of interfacial area. Finally, the soft lithography approach was also conducive for fabricating BPMs with different chemistries ranging from perfluorinated polymer backbones to alkaline stable poly(arylene) hydrocarbon polymers. These polymer chemistries are better suited for fuel cell and electrolysis applications. The BPM featuring the alkaline stable poly(terphenyl) anion exchange membrane had an onset potential of 0.84 V, which was near the thermodynamic limit, and was about 150 mV lower than a commercially available variant.

25 ENERGY STORAGE↗
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 OSTI2025

Long-Range Charge Transport Facilitated by Electron Delocalization in MoS 2 and Carbon Nanotube Heterostructures

Controlling charge transport at the interfaces of nanostructures is crucial for their successful use in optoelectronic and solar energy applications. Mixed-dimensional heterostructures based on single-walled carbon nanotubes (SWCNTs) and transition metal dichalcogenides (TMDCs) have demonstrated exceptionally long-lived charge-separated states. However, the factors that control the charge transport at these interfaces remain unclear. In this study, we directly image charge transport at the interfaces of single- and multilayered MoS 2 and (6,5) SWCNT heterostructures using transient absorption microscopy. We find that charge recombination becomes slower as the layer thickness of MoS 2 increases. This behavior can be explained by electron delocalization in multilayers and reduced orbital overlap with the SWCNTs, as suggested by nonadiabatic (NA) molecular dynamics (MD) simulations. Dipolar repulsion of interfacial excitons results in rapid density-dependent transport within the first 100 ps. Stronger repulsion and longer-range charge transport are observed in heterostructures with thicker MoS 2 layers, driven by electron delocalization and larger interfacial dipole moments. These findings are consistent with the results from NAMD simulations. Our results suggest that heterostructures with multilayer MoS 2 can facilitate long-lived charge separation and transport, which is promising for applications in photovoltaics and photocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Twisted Tin‐Chloride Perovskite Single‐Crystal Heterostructures

Self-assembly affords simpler synthetic routes to heterostructures compared with manual layer-by-layer stacking, yet controlling interlayer twist angles in a bulk solid remains an outstanding challenge. We report two new single-crystal heterostructures: (Sn 2 Cl 2 )(CYS) 2 SnCl 4 (CYS = + NH 3 (CH 2 ) 2 S – ; Sn_CYS) and (Sn 2 Cl 2 )(SeCYS) 2 SnCl 4 (SeCYS = + NH 3 (CH 2 ) 2 Se – ; Sn_SeCYS) synthesized in solution, with alternating perovskite and intergrowth layers. Notably, compared to the recently reported lead analog, (Pb 2 Cl 2 )(CYS) 2 PbCl 4 (Pb_CYS), the tin heterostructures feature a twist between the perovskite and intergrowth layers. We trace this twist to local distortions at the Sn centers, which change the interfacial lattice-matching requirements compared to those of the Pb analog. Electronic band structure calculations show that the striking differences in the relative energies of perovskite- and intergrowth-derived bands in Sn_CYS and Pb_CYS arise from structural and not compositional differences. The structural anisotropy of Sn_CYS is also reflected in a large in-plane photoluminescence linear anisotropy ratio. Interfacial strain further affords differential incorporation of Pb into the perovskite and intergrowth layers of the Sn heterostructures, resulting in redshifted optical absorption onsets. Thus, we posit that local structural distortions may be exploited to manipulate the twist angle and interfacial strain in bulk heterostructures, providing a new handle for tuning the band alignments of bulk quantum-well electronic structures.

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

Hot-Carrier Transfer at Photocatalytic Silicon/Platinum Interfaces

Interfacial charge transfer from silicon to heterogeneous catalysts plays a key role in silicon-based photoelectrochemical systems. In general, prior to interfacial charge transfer, carriers that are generated by photons with energies above the bandgap dissipate the excess kinetic energy via hot-carrier cooling, and such energy loss limits the maximum power conversion efficiency. The excess energy of hot-carriers, however, could be utilized through hot-carrier transfer from silicon to the catalysts, but such hot-carrier extraction has not yet been demonstrated. In this work, we exploit transient reflection spectroscopy to interrogate charge transfer at the interface between silicon and platinum. Additionally, quantitative modeling of the surface carrier kinetics indicates that the velocity of charge transfer from silicon to platinum exceeds 2.6 x 10 7 cm s -1 , corresponding to an average carrier temperature of extracted carriers of ~600 K, two times higher than the lattice temperature. The charge transfer velocity can be controllably reduced by inserting silica spacing layers between silicon and platinum.

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

Modeling the electrochemical behavior and interfacial junction profiles of bipolar membranes at solar flux relevant operating current densities

A 1-dimensional, multi-physics model that accounts for the migration and diffusion of solution species, electrostatics, and chemical reactions, in particular water dissociation (WD), at bipolar membrane (BPM) interfaces was developed to study the electrochemical behavior of bipolar membranes (BPMs) at solar flux relevant operating current densities (tens of mA cm -2 ). Significant partial current densities for WD were observed at BPM voltages much less than the equilibrium voltage, e.g., 59 mV × ΔpH from both experiments and modeling. The co-ion leakage across the BPM at pH differentials accounted for the early presence of the partial current density for WD. Two distinctive electric field dependent WD pathways, the un-catalyzed pathway and the catalyzed pathway, were quantitatively and parametrically studied to improve the turn-on potential of the BPM. The catalyzed pathway accounted for the majority of the partial current density for WD at low voltages, while the un-catalyzed pathway dominated the WD at relatively high voltages. Significant WD was observed only within the interfacial CL (<5 nm), in which a large electric field was present. To improve the electrochemical behavior and the turn-on potential of BPMs, the impacts of the pKa of the immobilized WD catalysts, the electric-field dependent rate constant, the thickness of the catalyst layer and fixed charge density in BPMs on the partial current densities for WD were studied systematically. In addition, the electrochemical behavior and concentration profiles of BPMs in a buffered electrolyte were studied and contrasted with those in an un-buffered electrolyte from both modeling and experiments.

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

Studying Interfacial Dark Reactions of Glyoxal and Hydrogen Peroxide Using Vacuum Ultraviolet Single Photon Ionization Mass Spectrometry

Aqueous secondary organic aerosol (aqSOA) formation from volatile and semivolatile organic compounds at the air–liquid interface is considered as an important source of fine particles in the atmosphere. However, due to the lack of in situ detecting techniques, the detailed interfacial reaction mechanism and dynamics still remain uncertain. In this study, synchrotron-based vacuum ultraviolet single-photon ionization mass spectrometry (VUV SPI-MS) was coupled with the System for Analysis at the Liquid Vacuum Interface (SALVI) to investigate glyoxal dark oxidation products at the aqueous surface. Mass spectral analysis and determination of appearance energies (AEs) suggest that the main products of glyoxal dark interfacial aging are carboxylic acid related oligomers. Furthermore, the VUV SPI-MS results were compared and validated against those of in situ liquid time-of-flight secondary ion mass spectrometry (ToF-SIMS). The reaction mechanisms of the dark glyoxal interfacial oxidation, obtained using two different approaches, indicate that differences in ionization and instrument operation principles could contribute to their abilities to detect different oligomers. Therefore, the mechanistic differences revealed between the VUV SPI-MS and ToF-SIMS indicate that more in situ and real-time techniques are needed to investigate the contribution of the air–liquid interfacial reactions leading to aqSOA formation.

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

The Role of Interfacial Thermal Resistance in Li-Ion Battery Thermal Management: Preprint

Temperature critically affects the performance, life and safety of lithium-ion batteries. Therefore, it is essential to understand heat generation and dissipation within individual battery cells and battery packs to plan a proper thermal management strategy. One of the key challenges is that interfacial heat transfer of a battery unit is difficult to quantify. The steady-state absolute method and the transient laser-flash-diffusivity method were employed to measure heat conductivities of battery layer stacks and individual battery layer separately. Results show flash diffusivity method gives higher thermal conductivity at both cross-plane and in-plane directions. The difference is primarily caused by interfacial thermal resistance so that it can be estimated by steady-state and transient measurements. To investigate the effects of interfacial thermal transport beyond individual cell level, a multiphysics battery model is used. The model is built upon a multi-scale multi-domain modeling framework for battery packs that accounts for the interplay across multiple physical phenomena. Benefits of a battery module using thermal management materials are quantified through numerical experiments. During a thermal runaway event, it is found interfacial thermal resistance can mitigate thermal runaway in a battery module by significantly reducing heat transfer between cells.

33 ADVANCED PROPULSION SYSTEMS↗
NASA NTRS2004

The Fluids and Combustion Facility

Microgravity is an environment with very weak gravitational effects. The Fluids and Combustion Facility (FCF) on the International Space Station (ISS) will support the study of fluid physics and combustion science in a long-duration microgravity environment. The Fluid Combustion Facility's design will permit both independent and remote control operations from the Telescience Support Center. The crew of the International Space Station will continue to insert and remove the experiment module, store and reload removable data storage and media data tapes, and reconfigure diagnostics on either side of the optics benches. Upon completion of the Fluids Combustion Facility, about ten experiments will be conducted within a ten-year period. Several different areas of fluid physics will be studied in the Fluids Combustion Facility. These areas include complex fluids, interfacial phenomena, dynamics and instabilities, and multiphase flows and phase change. Recently, emphasis has been placed in areas that relate directly to NASA missions including life support, power, propulsion, and thermal control systems. By 2006 or 2007, a Fluids Integrated Rack (FIR) and a Combustion Integrated Rack (CIR) will be installed inside the International Space Station. The Fluids Integrated Rack will contain all the hardware and software necessary to perform experiments in fluid physics. A wide range of experiments that meet the requirements of the international space station, including research from other specialties, will be considered. Experiments will be contained in subsystems such as the international standard payload rack, the active rack isolation system, the optics bench, environmental subsystem, electrical power control unit, the gas interface subsystem, and the command and data management subsystem. In conclusion, the Fluids and Combustion Facility will allow researchers to study fluid physics and combustion science in a long-duration microgravity environment. Additional information is included in the original extended abstract.

Kundu, Sampa↗
DOE OSTI2023

Chemical Design of Organic Interface Modifiers for Highly Efficient and Stable Perovskite Solar Cells

Perovskite solar cells (PSCs) have demonstrated rapid progress in their power conversion efficiencies (PCEs) - from 3.8% in 2009 to 25.7% in 2022 - and they have received considerable attention as a promising future photovoltaic (PV) technology. However, the operational stability of PSCs is still inadequate to satisfy the standards for commercial applications. Interface engineering has become one of the most important strategies to push PSCs' efficiency and stability for practical use. Among the various interface engineering approaches, organic interface modifiers (OIMs) have been frequently used by the PSC field to address the issues limiting PSC stability at high efficiency levels. In this perspective, the chemical structures of state-of-the-art OIMs are discussed, and their characteristics are reviewed, as well as the impact on device performance associated with key device interfaces (e.g., metal oxide/perovskite and organic transport layer/perovskite interfaces) from a chemical and materials engineering point of view is discussed. Finally, design considerations and the authors' perspective are discussed, on the basis of representative literature examples, for building new, customized organic OIMs to further improve PSC efficiency and stability toward commercialization.

14 SOLAR ENERGY↗
DOE OSTI2024

Computational Insights into Phase Equilibria Between Wide-Gap Semiconductors and Contact Materials

Novel wide-band-gap semiconductors are needed for next-generation power electronics, but there is a gap between a promising material and a functional device. Finding stable (metal) contacts is one of the major challenges that is currently dealt with mainly via trial and error. Herein, we computationally investigate the thermochemistry and phase coexistence at the junction between three wide-gap semiconductors, ..beta..-Ga2O3, GeO2, and GaN, and possible contact materials. The pool of possible contacts includes 47 elemental metals and a set of 4 common, n-type transparent conducting oxides (ZnO, TiO2, SnO2, and In2O3). We use first-principles thermodynamics to model the Gibbs free energies of chemical reactions as a function of gas pressure (pO2/pN2) and equilibrium temperature. We deduce whether a semiconductor/contact interface will be stable at relevant conditions or a chemical reaction between them is to be expected, possibly influencing the long-term reliability and performance of devices. We generally find that most elemental metals tend to oxidize or nitridize and form various interface oxide/nitride layers. Exceptions include select late- and post-transition metals and, in the case of GaN, also the alkali metals, which are predicted to exhibit stable coexistence, although in many cases at relatively low gas partial pressures. Similar is true for the transparent conducting oxides, for which, in most cases, we predict a preference toward forming ternary oxides when in contact with ..beta..-Ga2O3 and GeO2. The only exception is SnO2, which we find to form stable contacts with both oxides. Finally, we show how the same approach can be used to predict gas partial pressure vs temperature phase diagrams to help direct synthesis of ternary compounds. We believe these results provide a valuable guidance in selecting contact materials to wide-gap semiconductors and suitable growth conditions.

contact materials↗
DOE OSTI2020

Designing electrolytes with polymerlike glass-forming properties and fast ion transport at low temperatures

Significance Liquid electrolytes with thermophysical properties analogous to solid polymers, but with exceptional liquidlike ionic conductivities, are formed spontaneously when moderate amounts (≤1 M) of inorganic salts coordinate strongly with small molecules in a conventional aprotic solvent. Specifically, we report that electrolytes composed of the cyclic liquid ether, dioxolane (DOL), and containing the simple salt LiNO 3 are able to completely bypass the liquid → crystalline solid thermal transition, and to exhibit abnormally high bulk and interfacial ionic conductivities down to temperatures as low as −50 °C. Through physical, spectroscopic, and ion-transport measurements it is shown that strong interactions between LiNO 3 and DOL distort bonds in DOL, couple motions of individual solvent molecules, and lower the thermodynamic activity of the electrolyte.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effect of interfacial structures on phonon transport across atomically precise Si/Al heterojunctions

Phonons are important carriers of energy and information in many cryogenic devices used for quantum information science and in fundamental physics experiments such as dark matter detectors. In these systems phonon behavior can be dominated by interfaces, hence there is increasing demand for a more detailed understanding of interfacial phonon transport in relevant material systems. Previous studies have focused on understanding thermal transport over the entire phonon spectrum at and above room temperature. At ultra-low temperatures, however, knowledge is missing regarding athermal phonon behavior due to the challenge in modeling the extreme conditions in micro-scale, heterogeneous cryogenic systems, as well as extracting single-phonon information from a large ensemble. In this work, we delineate interfacial phonon transport using a combination of classical molecular dynamics (MD) and phonon wave packet simulations, to illustrate the consistency and differences between the ensemble- and single-phonon dynamics. We consider three single-crystal Si surface reconstructions --- (1×1), (v3×v3) and (7×7) --- and model both experimentally observed Si(1×1)/Al interfaces and hypothesized Si(v3×v3)/Al and Si(7×7)/Al interfaces. The overall interfacial thermal conductance calculated from non-equilibrium MD shows that for the Si(1×1)/Al system, the presence of Al twin grain boundaries can hinder phonon transport and reduce thermal conductance by 2--12% relative to single-crystal Al; whereas the Si (v3×v3) and (7×7) reconstructions can enhance it by 6--19%. Normal mode decomposition reveals that both the increase and decrease in conductance are related to inelastic phonon scattering. Single-phonon wave packet simulations show results consistent with NEMD, while further suggesting that phonon polarization conversion is significant even when elastic transmission dominates, and that the interfacial structures have anisotropic impacts on atomic vibrations along different lattice directions. Our findings suggest alternative perspectives in achieving selective phonon transport through controlling interfacial structures of materials with atomically-precise fabrication techniques, and that the phonon wave packet formalism is a potentially powerful method for developing a detailed understanding of non-equilibrium phenomena in the low-temperature limit.

Lu, Zexi↗
DOE OSTI2024

Colloquium : Sliding and pinning in structurally lubric 2D material interfaces

A plethora of two-dimensional (2D) materials have been introduced in physics and engineering in the past two decades. Their robust, membranelike sheets permit (mostly require) deposition, giving rise to solid-solid dry interfaces whose mobility, pinning, and general tribological properties under shear stress are currently being understood and controlled, both experimentally and theoretically. Here, in this Colloquium simulated case studies of twisted graphene systems are used as a prototype workhorse tool to demonstrate and discuss the general picture of 2D material interface sliding. First highlighted is the crucial mechanical difference, often overlooked, between small and large incommensurabilities, which corresponds to, for example, small and large twist angles in graphene interfaces. In both cases, focusing on flat, structurally lubric or “superlubric” geometries, the generally separate scalings with the area of static friction in pinned states and of kinetic friction during sliding are elucidated and reviewed, tangled as they are with the effects of velocity, temperature, load, and defects. The roles of island boundaries and elasticity are also discussed, and compared when possible to results in the literature for systems other than graphene. It is proposed that the resulting picture of pinning and sliding should be applicable to interfaces in generic 2D materials that are of importance for the physics and technology of existing and future bilayer and multilayer systems.

2-dimensional systems↗
DOE OSTI2020

Nanometal-Interconnected Carbon Conductors (NICCS) for Advanced Electric Machines (RIT Final Technical Report)

Recent advancements in carbon nanotube (CNT) research have enabled lightweight, conductive wires as a transformative technology. Metal-carbon nanotube (CNT) hybrid conductors aim to combine the high conductivity of traditional metals with the low mass and temperature coefficient of resistance (TCR) of carbon nanotubes. The high conductivity of copper makes it a promising candidate to combine with CNTs in a hybrid structure, but there is limited physical and electrical interaction between copper and CNTs. The use of an interfacial layer offers one method of improving the interconnection of a Cu-CNT hybrid conductor. Over the course of this grant, a joule heating-driven chemical vapor deposition (CVD) technique was developed to deposit nanometal seeds throughout a porous, low-density (0.12 g/cm 3 , ~10 tex or mg/m) CNT roving template. Modification of the applied current to the CNT roving allows for the tuning of depositions towards either hot-spot site-specificity or overall uniformity. The effects of temperature, pressure, precursor mass, and the interval of applied current were investigated, demonstrating nanometal depositions ranging from less than 5 % w/w to over 85 % w/w. The versatility of CVD allows for a wide variety of metals to be deposited including copper, titanium, nickel, silver, tungsten, palladium, platinum, ruthenium, rhodium, and iridium. One preferred demonstration involved using platinum depositions to improve the electrical properties of metal-seeded CNTs across all mass loadings studied. Moreover, when the metal-seeded CNT wires were electroplated with copper, densified, and annealed under hydrogen/argon; the result was a Cu-CNT hybrid conductor with the highest conductivities reported to date. The good interconnection of the metal and CNT portions results in a stable conductor. An electrical conductivity of 16-20 MS/m was achieved for multiple Cu-CNT hybrid conductors at 150 °C, which exceeds the program goal for conductivity of greater than 15 MS/m for a 1 m long CNT wire. Overall, the research outcomes from the project showed improvements in CNT wire fabrication from roll-to-roll CVD grown carbon nanotube wires using nanometal interconnects to bridge CNT-to-CNT junctions, thus mitigating network contact resistances. Advanced nanometal interconnected carbon conductors (NICCs) were developed as a means to achieve novel light-weight wiring appropriate for applications that require the conductivity of metallic (i.e., Cu, Al, etc.) wires at elevated temperatures. High conductivity, low TCR electrical conductors such as the nanometal interconnected Cu-CNT hybrids have numerous future applications towards high efficiency motors, generators, and transformers. Specifically, the advanced wires have the ability to operate at lower resistance during conditions for standard electric motors at 150 °C, which would improve the electrical efficiency while lowering energy needs.

36 MATERIALS SCIENCE↗