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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 559 records · Page 31
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Lifetime and linewidth of individual quantum dots interfaced with graphene

Here, we report on luminescence lifetimes and linewidths from an array of individual quantum dots (QDs) that were either interfaced with graphene surface guides or dispersed on aluminum electrodes. The observed fluorescence quenching is consistent with screening by charge carriers. Fluorescence quenching is typically mentioned as a sign that chromophores are interfacing with a conductive surface (metal or graphene); we find that the QDs interfaced with the metal film exhibit shortened lifetime and line-broadening but not necessarily fluorescence quenching as the latter may be impacted by molecular concentration, reflectivity and conductor imperfections. We also comment on angle-dependent lifetime measurements, which we postulate depend on the specifics of the local density-of-states involved.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS1974

Preparation and evaluation of thin-film sodium tungsten bronzes

Thin films of sodium tungsten bronze (NaxWO3) were investigated as reversible sodium ion electrodes for solid electrolytes. The films were made by electron beam evaporation of the three phases, W metal, Na2WO4, and WO3, followed by sintering. The substrates were sodium beta alumina disks and glass slides. X-ray diffraction analyses of the films showed that sintering in dry nitrogen with prior exposure to air lead to mixed phases. Sintering in vacuum with no air exposure produced tetragonal I bronze with a nominal composition of Na0.31WO3, single phase within the limits of X-ray diffraction detectability. The films were uniform and adherent on sodium beta alumina substrates. The ac and dc conductivities of the beta alumina were measured with the sodium tungsten bronze films as electrodes. These experiments indicated that the tetragonal I bronze electrodes were not completely reversible. This may have resulted from sodium ion blocking within the bronze film or at the bronze beta alumina interface. Methods for attempting to make more completely reversible electrodes are suggested.

Kautz, H. E.↗
NASA NTRS1980

Testing EKG electrodes on-line

Simple test instrument allows electrocardiograph operator to check individual electrodes while they are attached to subject. Simply by rotating switch and observing meter, operator verifies that each electrode is not short-circuited or open-circuited and does not present excessive contact resistance at its interface with skin. Instrument also makes it convenient to check electrode cables that are subject to frequent bending and wear, such as cables used on patients who are exercising.

Crosier, W. G.↗
DOE OSTI2024

Effect of ZnO and PEDOT:PSS charge selective layers on photovoltage of cuprous oxide (Cu 2 O) heterojunction solar cells

Electrochemical deposition (ECD) of Cu 2 O provides a scalable and low temperature pathway to solar cells with a theoretical high energy conversion efficiency of 23%, based on the 2.0–2.2 eV band gap of Cu 2 O. However, existing ECD-Cu 2 O devices are plagued by poor crystallinity and low selectivity of the electron and hole transport layers. Here we use Vibrating Kelvin Probe Surface Photovoltage Spectroscopy (VKP-SPV) to probe the charge transfer selectivity in FTO/ZnO/Cu 2 O/PEDOT:PSS/Ni heterojunction solar cells. Selective electron extraction is achieved at the ZnO back contact to Cu 2 O, as confirmed by a negative surface photovoltage signal. While the uncoated Cu 2 O surface is electron-selective due to the formation of a hole depletion layer, spin coating of a PEDOT:PSS film turns it into a hole-selective interface. After adding nickel metal ink top electrodes, functional 1.0 cm 2 solar cells with power conversion efficiency (PCE) of up to 0.07%, 195 mV open-circuit voltage, and 1.28 mA cm –2 short-circuit photocurrent are achieved. The photovoltaic performance is higher for aluminum doped zinc oxide (AZO) substrates than for fluorine doped tin oxide (FTO) due to the presence of a n-/p-junction that further increases the electron selectivity of the AZO/ZnO/Cu 2 O contacts. Overall, this work demonstrates the first application of PEDOT:PSS as a hole transport layer (HTL) for Cu 2 O and the use of VKP-SPV to measure the photovoltage contributions of the Cu 2 O interfaces. Furthermore, the ability to fabricate Cu 2 O solar cells at near room temperature without the use of vacuum methods or rare elements is an important step towards a scalable Cu 2 O PV technology.

14 SOLAR ENERGY↗
DOE OSTI2020

In Situ Formation of Li 3 P Layer Enables Fast Li + Conduction across Li/Solid Polymer Electrolyte Interface

Abstract Solid‐state polymer electrolytes provide better flexibility and electrode contact than their ceramic counterparts, making them a worthwhile pursuit for all‐solid‐state lithium‐metal batteries. However, their large Li/solid state electrolyte interfacial resistance, small critical current density, and rapid lithium dendrite growth during cycling still limit their viability. Owing to these restrictions, all‐solid‐state cells with solid polymer electrolytes must be cycled above room‐temperature and with a small current density. These problems can be mitigated with an in situ formed artificial solid electrolyte interphase that rapidly conducts Li + ions. Herein, a Li 3 P layer formed in situ at the Li‐metal/solid polymer electrolyte interphase is reported that significantly reduces the electrode/electrolyte interfacial resistance. Additionally, this layer increases the wettability of the solid polymer by the metallic lithium anode, allowing for the critical current density of lithium symmetric cells to be doubled by homogenizing the current density at the interface. All‐solid‐state Li/Li symmetric cells and Li/LiFePO 4 cells with the Li 3 P layer show improved cycling performance with a high current density.

Wu, Nan↗
DOE OSTI2017

Origin of Low-Energy Spurious Peaks in Spectroscopic Measurements With Silicon Detectors

We report that when an uncollimated radioactive X-ray source illuminates a silicon PIN sensor, some ionizing events are generated in the nonimplanted gap between the active area of the sensor and the guard rings (GRs). Carriers can be collected by floating electrodes, i.e., electron accumulation layers at the silicon/oxide interface, and floating GRs. The crosstalk signals generated by these events create spurious peaks, replicas of the main peaks at either lower amplitude or of opposite polarity. Lastly, we explain this phenomenon as crosstalk caused by charge collected on these floating electrodes, which can be analyzed by means of an extension of Ramo theorem.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Fundamental Investigations of Mechanical and Chemical Degradation Mechanisms in Lithium Ion Battery Materials (Final Technical Report)

The objective of our effort under the DOE EPSCoR Implementation grant is to establish a comprehensive and internationally recognized research program at Brown University and University of Rhode Island in understanding degradation mechanisms and to improve the cycle and calendar life of lithium ion battery (LIB) materials. A series of basic investigations are undertaken to characterize the mechanical and chemical degradation mechanisms, which can help enable new higher capacity and longer lasting electrode designs. Controlling mechanical and chemical degradation is the primary challenge in developing the next generation of higher energy density batteries. The development of failure resistant battery microstructures will require a fundamental understanding of the evolution of stress, deformation, damage, and electrochemistry in battery materials during cyclic charging and discharging. In addition, controlling the reactions at the electrode/electrolyte interface is critical for the formation of a stable SEI layer. We address these issues through a combination of controlled experiments on model battery materials and practical composite electrodes, together with multi-scale computations. Our effort is organized into three focus areas that encompass many critical challenges in Lithium Ion Battery Technologies: (i) Mechanical properties, fracture and damage in electrode materials; (ii) Chemistry and Mechanics of Solid Electrolyte Interphase (SEI); (iii) Mechanical and Chemical Integrity of Solid-Solid Interfaces in Practical Electrodes.

25 ENERGY STORAGE↗
DOE OSTI2018

Aqueous vs. nonaqueous Zn-ion batteries: consequences of the desolvation penalty at the interface

Zinc ion batteries using metallic zinc as the negative electrode have gained considerable interest for electrochemical energy storage, whose development is crucial for the adoption of renewable energy technologies, as zinc has a very high volumetric capacity (5845 mA h cm -3 ), is inexpensive and compatible with aqueous electrolytes. However, the divalent charge of zinc ions, which restricts the choice of host material due to hindered solid-state diffusion, can also pose a problem for interfacial charge transfer. We report our findings on reversible intercalation of up to two Zn 2+ ions in layered V 3 O 7 ·H 2 O. This material exhibits very high capacity and power (375 mA h g -1 at a 1C rate, and 275 mA h g -1 at an 8C rate) in an aqueous electrolyte compared to a very low capacity and slow rate capabilities in a nonaqueous medium. Operando XRD studies, together with impedance analysis, reveal solid solution behavior associated with Zn 2+ -ion diffusion within a water monolayer in the interlayer gap in both systems, but very sluggish interfacial charge transfer in the nonaqueous electrolyte. This points to desolvation at the interface as a major factor in dictating the kinetics. Temperature dependent impedance studies show high activation energies associated with the nonaqueous charge transfer process, identifying the origin of poor electrochemical performance.

25 ENERGY STORAGE↗
DOE OSTI2021

Degradation Diagnostics from the Subsurface of Lithium-Ion Battery Electrodes

Despite the long-established rocking-chair theory of lithium-ion batteries (LIBs), developing novel characterization methodology with higher spatiotemporal resolution facilitates a better understanding of the solid electrolyte interphase studies to shape the reaction mechanisms. In this work, we develop a Xenon ion plasma focused ion beam (Xe + PFIB)-based characterization technique to probe the cross-sectional interface of both ternary cathode and graphite anode electrodes, with the focus on revealing the chemical composition and distribution underneath the electrode surface by in-depth analysis of secondary ions. Particularly, the lithium fluoride is detected in the pristine cathode prior to contact with the electrolyte, reflecting that the electrode degradation is in the form of the loss of lithium inventory during electrode preparation. This degradation is related to the hydrolysis of the cathode material and the decomposition of the PVDF binder. Here, through the quantitative analysis of the transition-metal degradation products, manganese is found to be the dominant element in the newly formed inactive fluoride deposition on the cathode, while no transition metal signal can be found inside the anode electrode. These insights at high resolution implemented via a PFIB-based characterization technique not only enrich the understanding of the degradation mechanism in the LIBs but also identify and enable a high-sensitivity methodology to obtain the chemical survey at the subsurface, which will help remove the capacity-fade observed in most LIBs.

25 ENERGY STORAGE↗
DOE OSTI2019

Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating

To improve electric vehicle market acceptance, the charge time of their batteries should be reduced to 10–15 minutes. However, achieving 4C to 6C charge rates with today’s batteries is only possible for cells with thin electrodes coming at the expense of low energy density and high battery manufacturing cost. An electrochemical model is validated versus high rate charge data for cells with several loadings. The model elucidates that the main limitations for high energy density cells are poor electrolyte transport resulting in salt depletion within the anode and Li plating at the graphite/separator interface. Next, the model is used to understand what future electrode and electrolyte properties can help enable 4C and 6C charging. Ideally, future electrolytes would be identified with 2X conductivity, 3–4X diffusivity, and transference number of 0.5–0.6. Alternatively charging at elevated temperatures enhances electrolyte transport by 1.5X conductivity and 2–3X diffusivity with a negligible effect on transference number. Another effective strategy to enable 4C and 6C charging is reducing electrode tortuosity. Conversely, increasing electrode porosity and negative/positive ratio are ineffective strategies to improve fast charge capability.

Batteries↗
DOE OSTI2023

Microscale Electrochemical Corrosion of Uranium Oxide Particles

Understanding the corrosion of spent nuclear fuel is important for the development of long-term storage solutions. However, the risk of radiation contamination presents challenges for experimental analysis. Adapted from the system for analysis at the liquid–vacuum interface (SALVI), we developed a miniaturized uranium oxide (UO 2 )-attached working electrode (WE) to reduce contamination risk. To protect UO 2 particles in a miniatured electrochemical cell, a thin layer of Nafion was formed on the surface. Atomic force microscopy (AFM) shows a dense layer of UO 2 particles and indicates their participation in electrochemical reactions. Particles remain intact on the electrode surface with slight redistribution. X-ray photoelectron spectroscopy (XPS) reveals a difference in the distribution of U(IV), U(V), and U(VI) between pristine and corroded UO 2 electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO 2 oxidation can be studied using these cells. Our observations of U(V) in the micro-electrode due to the selective semi-permeability of Nafion suggest that interfacial water plays a key role, potentially simulating a water-lean scenario in fuel storage conditions. This novel approach offers analytical reproducibility, design flexibility, a small footprint, and a low irradiation dose, while separating the α-effect. This approach provides a valuable microscale electrochemical platform for spent fuel corrosion studies with minimal radiological materials and the potential for diverse configurations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Tunneling field-effect junctions with WS 2 barrier

Transition metal dichalcogenides (TMDCs), with their two-dimensional structures and sizable bandgaps, are good candidates for barrier materials in tunneling field-effect junctions (TFEJ) formed from atomic precision vertical stacks of graphene and insulating crystals of a few atomic layers in thickness. Here we report first-principles study of the electronic properties of the Graphene/WS 2 /Graphene sandwich structure revealing strong interface effects on dielectric properties and predicting a high ON/OFF ratio with an appropriate WS 2 thickness and a suitable range of the gate voltage. Both the band spin-orbit coupling splitting and the dielectric constant of the WS 2 layer depend on its thickness when in contact with the graphene electrodes, indicating strong influence from graphene across the interfaces. The dielectric constant is significantly reduced from the bulk WS 2 value. The effective barrier height varies with WS 2 thickness and can be tuned by a gate voltage. These results are critical for future nanoelectronic device applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Vibrational Probe at the Electrochemical Interface: Dependence on Plasmon Coupling and Potential of the Lineshape in Two-Dimensional Infrared Spectroscopy

Two-dimensional infrared spectroscopy of vibrational probes at an electrode surface shows promise for studying the structural dynamics at an active electrochemical interface. This interface is a complex environment where the solution structures in response to the applied potential. A strategy for achieving the necessary monolayer sensitivity is to use a plasmonically active electrode, which enhances the electromagnetic fields that produce the spectroscopic response. Here, in this study, we show how the coupling between the plasmon and the vibrations of the molecular monolayer impacts the FTIR and 2D IR spectroscopy, with an emphasis on the electrochemical potential difference spectra. We show how mixing between the vibrational and plasmonic states gives rise to the distortions that are observed in these measurements. This provides an important step toward 2D IR measurements of vibrational probes at the electrochemical interface as a tool for probing the structural dynamics in the double layer.

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

Theoretical Modeling of Electrochemical Proton-Coupled Electron Transfer

Proton-coupled electron transfer (PCET) plays an essential role in a wide range of electrocatalytic processes. Here, a vast array of theoretical and computational methods have been developed to study electrochemical PCET. These methods can be used to calculate redox potentials and pKa values for molecular electrocatalysts, proton-coupled redox potentials and bond dissociation free energies for PCET at metal and semiconductor interfaces, and reorganization energies associated with electrochemical PCET. Periodic density functional theory can also be used to compute PCET activation energies and perform molecular dynamics simulations of electrochemical interfaces. Various approaches for maintaining a constant electrode potential in electronic structure calculations and modeling complex interactions in the electric double layer (EDL) have been developed. Theoretical formulations for both homogeneous and heterogeneous electrochemical PCET spanning the adiabatic, nonadiabatic, and solvent-controlled regimes have been developed and provide analytical expressions for the rate constants and current densities as functions of applied potential. The quantum mechanical treatment of the proton and inclusion of excited vibronic states have been shown to be critical for describing experimental data, such as Tafel slopes and potential dependent kinetic isotope effects. The calculated rate constants can be used as input to microkinetic models and voltammogram simulations to elucidate complex electrocatalytic processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Water-Activated VOPO 4 for Magnesium Ion Batteries

Rechargeable Mg batteries, using high capacity and dendrite-free Mg metal anodes, are promising energy storage devices for large scale smart grid due to low cost and high safety. However, the performance of Mg batteries is still plagued by the slow reaction kinetics of their cathode materials. Recent discoveries demonstrate that water in cathode can significantly enhance the Mg-ion diffusion in cathode by an unknown mechanism. Here, we propose the water-activated layered-structure VOPO 4 as a novel cathode material and examine the impact of water in electrode or organic electrolyte on the thermodynamics and kinetics of Mg-ion intercalation/deintercalation in cathodes. Electrochemical measurements verify that water in both VOPO 4 lattice and organic electrolyte can largely activate VOPO 4 cathode. Thermodynamic analysis demonstrates that the water in the electrolyte will equilibrate with the structural water in VOPO 4 lattice, and the water activity in the electrolyte alerts the mechanism and kinetics for electrochemical Mg-ion intercalation in VOPO 4 . Theoretical calculations and experimental results demonstrate that water reduces both the solid-state diffusion barrier in the VOPO 4 electrode and the desolvation penalty at the interface. To achieve fast reaction kinetics, the water activity in the electrolyte should be larger than 10 –2 . The proposed activation mechanism provides guidance for screening and designing novel chemistry for high performance multivalent-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Impact of surface hydrophilicity on the ordering and transport properties of bicontinuous microemulsions

Microemulsions (MEs) have many industrial applications, where recent developments have shown that MEs can be utilized for electrochemical applications, including potentially in redox flow batteries. However, understanding the structure and dynamics of these systems, including at a surface, is needed to direct and rationally control their electrochemical behavior. While bulk solution measurements have provided insight into their structure, their assembly at an interface also impacts the electron (to the electrode) and ion (across the surfactant) charge transfer processes in the system. To address this shortcoming, neutron reflectivity experiments and molecular simulations have been completed that document the near surface structure of a series of deuterated water (D 2 O)/polysorbate-20/toluene MEs on hydrophilic and amphiphilic surfaces. These results show that the microemulsions form complex layered structures near a hard electrode surface, where most layers are not purely one component. Decreasing the D 2 O concentration in the ME increases the number of and purity of the layers established on the solid surface. These lamellar-type layers transition from the surface to the bulk microemulsion as a series of mixed layers (i.e., containing oil, water, and surfactant) that are consistent with perforated lamellae. Additionally, these mixed lamellae appear to become more perforated with oil and water pathways on an amphiphilic surface. Furthermore, the purity and thickness of these layers will influence the accessibility of an electrode by redox active species, as well as ion transport required to satisfy the electroneutrality condition.

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

Energy conversion and transport in molecular-scale junctions

Molecular-scale junctions (MSJs) have been considered the ideal testbed for probing physical and chemical processes at the molecular scale. Due to nanometric confinement, charge and energy transport in MSJs are governed by quantum mechanically dictated energy profiles, which can be tuned chemically or physically with atomic precision, offering rich possibilities beyond conventional semiconductor devices. While charge transport in MSJs has been extensively studied over the past two decades, understanding energy conversion and transport in MSJs has only become experimentally attainable in recent years. As demonstrated recently, by tuning the quantum interplay between the electrodes, the molecular core, and the contact interfaces, energy processes can be manipulated to achieve desired functionalities, opening new avenues for molecular electronics, energy harvesting, and sensing applications. This Review provides a comprehensive overview and critical analysis of various forms of energy conversion and transport processes in MSJs and their associated applications. We elaborate on energy-related processes mediated by the interaction between the core molecular structure in MSJs and different external stimuli, such as light, heat, electric field, magnetic field, force, and other environmental cues. Key topics covered include photovoltaics, electroluminescence, thermoelectricity, heat conduction, catalysis, spin-mediated phenomena, and vibrational effects. Furthermore, the review concludes with a discussion of existing challenges and future opportunities, aiming to facilitate in-depth future investigation of promising experimental platforms, molecular design principles, control strategies, and new application scenarios.

Charge transport↗
DOE OSTI2021

Electrochemistry of the NaI-AlBr 3 Molten Salt System: A Redox-Active, Low-Temperature Molten Salt Electrolyte

NaI-AlBr 3 is a very appealing low melting temperature (<100 °C), salt system for use as an electrochemically-active electrolyte. This system was investigated for its electrochemical and physical properties with focus to energy storage considerations. A simple phase diagram was generated; at >100 °C, lower NaI concentrations had two partially miscible liquid phases, while higher NaI concentrations had solid particles. Considering the fully molten regime, electrical conductivities were evaluated over 5–25 mol% NaI and 110 °C–140 °C. Conductivities of 6.8–38.9 mS cm −1 were observed, increasing with temperature and NaI concentration. Effective diffusion coefficients of the I − /I 3 − redox species were found to decrease with both increasing NaI concentration and increasing applied potential. Regardless, oxidation current density at 3.6 V vs Na/Na + was observed to increase with increasing NaI concentration over 5–25 mol%. Finally, the critical interface between the molten salt electrolyte and electrode materials was found to significantly affect reaction kinetics. When carbon was used instead of tungsten, an adsorbed species, most likely I 2 , blocked surface sites and significantly decreased current densities at high potentials. This study shows the NaI-AlBr 3 system offers an attractive, low-temperature molten salt electrolyte that could be useful to many applied systems, though composition and electrode material must be considered.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗