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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 631 records · Page 35

Formation of multi-charged ion beams by focusing effect of mid-electrode on electron cyclotron resonance ion source

We are constructing a tandem type electron cyclotron resonance ion source (ECRIS) and a beam line for extracting ion beams. The ion beam is extracted from the second stage by an accel-decel extraction system with a single-hole and the ion beam current on each electrode is measured. The total ion beam current is measured by a faraday cup downstream the extraction electrodes. We measure these currents as a function of the mid-electrode potential. We also change the gap length between electrodes and perform similar measurement. The behaviors of these currents obtained experimentally against the mid-electrode potential show qualitatively good agreement with a simple theoretical consideration including sheath potential effects. The effect of mid-electrode potential is very useful for decreasing the beam loss for enhancing ion beam current extracted from ECRIS.

43 PARTICLE ACCELERATORS↗

Atomically flat La-silicate/Si interface using tungsten carbide gate electrode with nano-sized grain

Interface properties of La-silicate gate dielectrics on Si substrates with W or nano-sized grain W{sub 2}C gate electrodes have been investigated. A low interface state density of 2.5 × 10{sup 11} cm{sup −2}/eV has been achieved with W{sub 2}C gate electrodes, which is one third of those with W gate electrode. An interface roughness of 0.33 nm with spatial frequency comparable to the grain size of W gate electrode has been observed. Besides, an atomically flat interface of 0.12 nm has been obtained with W{sub 2}C gate electrode. The origin of flat interface may be attributed to the elimination of inhomogeneous stress by grains in metal electrode.

36 MATERIALS SCIENCE↗

Influence of finite geometrical asymmetry of the electrodes in capacitively coupled radio frequency plasma

Capacitively coupled radio frequency (CCRF) plasmas are widely studied in last decades due to the versatile applicability of energetic ions, chemically active species, radicals, and also energetic neutral species in many material processing fields including microelectronics, aerospace, and biology. A dc self-bias is known to generate naturally in geometrically asymmetric CCRF plasma because of the difference in electrode sizes known as geometrical asymmetry of the electrodes in order to compensate electron and ion flux to each electrode within one rf period. The plasma series resonance effect is also come into play due to the geometrical asymmetry and excited several harmonics of the fundamental in low pressure CCRF plasma. In this work, a 13.56 MHz CCRF plasma is studied on the based on the nonlinear global model of asymmetric CCRF discharge to understand the influences of finite geometrical asymmetry of the electrodes in terms of generation of dc self-bias and plasma heating. The nonlinear global model on asymmetric discharge has been modified by considering the sheath at the grounded electrode to taking account the finite geometrical asymmetry of the electrodes. The ion density inside both the sheaths has been taken into account by incorporating the steady-state fluid equations for ions considering that the applied rf frequency is higher than the typical ion plasma frequency. Details results on the influences of geometrical asymmetry on the generation of dc self-bias and plasma heating are discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

An effect of the electrode material on space charge relaxation in ferroelectric copolymers of vinylidene fluoride

Processes of relaxation of space charges formed by impurities carriers in isotropic films of vinylidene fluoride and tetrafluoroethylene copolymers of the composition 71/29 and 94/6 were studied. Al and Au symmetric electrodes deposited by evaporation in vacuum have been used. In the case of Al electrodes at temperatures above 100 °C, giant low frequency dielectric dispersion was observed, while it is absent in films with Au electrodes. Causes of this phenomenon were studied by the X-ray photoelectron spectroscopy. It was shown that at Al deposition, new functional groups, such as Al-C, Al-F, and Al{sub 2}O{sub 3}, which are not characteristic of the copolymer film surface, formed. They were supposed to be traps for impurity carriers and because of this the electrode became partially blocked. This led to appearance of the giant electrode polarization on the metal-polymer boundary, which did not take place in the case of Au electrodes. Parameters of the Au4f line for the copolymer with different contents of fluorine atoms in the chain were analyzed. An increase in the number of these atoms was shown to result in the line shift to higher energies. This phenomenon was associated with an increase in the shift of the electron density from Au atoms to the F ones which has a high affinity to electrons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Electrode chemistry impact on retention performance of ferroelectric hafnium zirconium oxide (Hf 0.5 Zr 0.5 O 2−x ) capacitors

Polarization retention of 10 nm thick ferroelectric hafnium zirconium oxide (Hf 0.5 Zr 0.5 O 2−x , HZO) capacitors with W and TaN electrodes is investigated over temperatures ranging from 85 to 150 °C. Same state and opposite state polarization margins for devices with W electrodes show minimal retention loss after 10 5 at 150 °C. The devices capped with TaN electrodes show excellent same state retention, but the opposite state polarization margin in the TaN-electrode devices displays 40% retention loss at 150 °C after 10 5 s. The TaN-capped devices exhibit a more pronounced imprint, which is attributed to an increased oxygen vacancy content (compared to W-capped devices). The increased oxygen vacancy content in the TaN-capped devices is supported by photoluminescence and leakage current measurements. In addition, TaN-capped devices have chemically diffuse electrode–HZO interfaces; more abrupt interfaces are present in the W-capped devices. The presence of interfacial phases in the TaN-capped devices may lead to larger depolarization fields due to reduced charge screening. The results from this study provide further evidence that for HZO ferroelectric devices the electrode can significantly impact polarization retention behavior due to differences in oxygen vacancy concentration and formation of non-ferroelectric interfacial layers.

36 MATERIALS SCIENCE↗

Method of Measuring the Diffusion Resistance of the Structures of Porous Electrode Materials Based on a Proton-Conducting Ionomer and Carbon Nanomaterials

A method has been developed for measuring the oxygen mass-transport resistance of porous electrodes based on micro- and nanostructures of a Nafion proton-conducting ionomer, Pt/C, and carbon nanowires with the ultrahigh porosity. The method suggests measuring the limit oxygen electroreduction current density at the controlled oxygen flow through an electrochemical system and calculating the oxygen mass transport resistance using the ratio based on the Fick’s law. The method has been used to study the mass-transport loss of a membrane-electrode assembly electrode and electrode material based on a rotating disk electrode and can be applied in the development of new electrodes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Extreme Fast Charging: Effect of Positive Electrode Material on Crosstalk

Extreme fast charging (XFC) is a key requirement for the adoption of battery-based electric vehicles by the transportation sector. However, XFC has been shown to accelerate degradation, causing the capacity, life, and safety of batteries to deteriorate. We tested cells containing five positive electrode chemistries, LFP (olivine structure), LMO (spinel), LCO (layered), NMC811 (layered) and NCA (layered), using fast-charging protocols. After testing, the negative electrodes from cells containing positive electrodes crystallizing with a layered structure were found to have more lithium deposited on their surfaces. Further, those crystallizing with a layered structure also tended to have a larger increase in impedance than those crystallizing with a spinel or olivine structure. Characterization of the negative electrodes by X-ray photoelectron spectroscopy showed that using the concentrations of LiF and Li x PO y F z as metrics, the concentration of LiF in the SEI from the cell with different positive electrodes is LFP > LMO > LCO ~ NMC811 > NCA; and for Li x PO y F z , the order is LMO > LFP > NCA > NMC811 > LCO. Clearly, the positive-electrode material was influencing the amounts of these materials formed.

25 ENERGY STORAGE↗

Electrode Blocking Due to Redox Reactions in Aluminum Chloride-Sodium Iodide Molten Salts

Iodide redox reactions in molten NaI/AlCl 3 are shown to generate surface-blocking films, which may limit the useful cycling rates and energy densities of molten sodium batteries below 150 °C. An experimental investigation of electrode interfacial stability at 110 °C reveals the source of the reaction rate limitations. Electrochemical experiments in a 3-electrode configuration confirm an increase of resistance on the electrode surface after oxidation or reduction current is passed. Using chronopotentiometry, chronoamperometry, cyclic voltammetry, and electrochemical impedance spectroscopy, the film formation is shown to depend on the electrode material (W, Mo, Ta, or glassy carbon), as well as the Lewis acidity and molar ratio of I − /I 3 − in the molten salt electrolytes. These factors impact the amount of charge that can be passed at a given current density prior to developing excessive overpotential due to film formation that blocks the electrode surface. The results presented here guide the design and use of iodide-based molten salt electrolytes and electrode materials for grid scale battery applications.

25 ENERGY STORAGE↗

Morphological Influence in Lithium-Ion Battery 3D Electrode Architectures

The performance of lithium-ion batteries is limited by suboptimal energy density and power capability. A feasible approach is designing 3D electrode architectures where lithium ion transport in the electrolyte and active material can be optimized for improving the energy/power density. In this study, the influence of active material morphology and 3D electrode configurations is investigated with particular emphasis on solid-state transport and resulting implications on the performance. In this paper, a morphology-detailed computational modeling is presented which simulates lithium transport in disparate 3D electrode configurations. The resulting lithium concentration in the 3D electrode constructs during discharging, relaxation, and charging process reveal a local sate of charge map. This is correlated with the electrode performance. Finally, this study demonstrates the role of active particle morphology and 3D architecture on the electrode relaxation behavior, which determines the resulting concentration gradient and performance.

25 ENERGY STORAGE↗

A Multifunctional Isostructural Bilayer Oxygen Evolution Electrode for Durable Intermediate-Temperature Electrochemical Water Splitting

The overarching goal of the proposed research is to address SOEC’s degradation problem by advancing a new isostructural highly electrocatalytically active bilayer oxygen evolution reaction (OER) electrode, consisting of a LSCF (La 1-x Sr x Co 1-y Fe y O 3-δ ) core and a SCT (SrCo 0.9 Ta 0.1 O 3-δ ) shell, to achieve high and sustainable rate of oxygen evolution matching operating current densities without encountering delamination. To realize this goal, the project has adopted a combined experimental and theoretical approach to conduct research in the following six areas closely associated with SOPO tasks: 1) Development of electrocatalytically active bilayer oxygen electrodes (SOPO task-1) 2) Development of new symmetric three electrode cell (STEC) methodology to extract electrokinetic data of oxygen electrodes (SOPO task-2) 3) Quantification of electrokinetics of bilayer oxygen electrodes and correlation with degradation and delamination (SOPO task-2) 4) Performances of bilayer oxygen electrodes under fuel cells and electrolyzers modes (SOPO task-3) 5) Microscale modeling of oxygen electrode/electrolyte interface in solid oxide electrolysis cells (SOPO task-4) 6) Prediction of crack growth rate at oxygen electrode/electrolyte interface in solid oxide electrolysis cells (SOPO task-4)

08 HYDROGEN↗

Thin Film Electrodes with an Integral Current Collection Grid for Use with Solid Electrolytes

Thin film, high performance electrodes which can operate in high temperature environments are necessary for many devices which use a solid electrolyte. Electrodes of rhodium-tungsten alloy have been deposited on solid electrolyte using photolytic chemical vapor deposition (PCVD). A technique for depositing electrodes and current collection grids simultaneously has been developed using the prenucleation characteristics of PCVD. This technique makes it possible to fabricate electrodes which allow vapor transport through the thin (<1 (micro)m) portions of the electrode while integral thick grid lines improve the electronic conductivity of the electrode, thus improving overall performance.

thin film electrodes solid electrolyte vapor depos↗

Transparent Electrodes for Efficient Optoelectronics

With the development of new generations of optoelectronic devices that combine high performance and novel functionalities (e.g., flexibility/bendability, adaptability, semi or full transparency), several classes of transparent electrodes have been developed in recent years. These range from optimized transparent conductive oxides (TCOs), which are historically the most commonly used transparent electrodes, to new electrodes made from nano‐ and 2D materials (e.g., metal nanowire networks and graphene), and to hybrid electrodes that integrate TCOs or dielectrics with nanowires, metal grids, or ultrathin metal films. Here, the most relevant transparent electrodes developed to date are introduced, their fundamental properties are described, and their materials are classified according to specific application requirements in high efficiency solar cells and flexible organic light‐emitting diodes (OLEDs). This information serves as a guideline for selecting and developing appropriate transparent electrodes according to intended application requirements and functionality.

Morales‐Masis, Monica↗

“Top-Down” Li Deposition Pathway Enabled by an Asymmetric Design for Li Composite Electrode

Designing Li composite electrodes with host frameworks for accommodating Li metal has been considered to be an effective approach to suppress Li dendrites. Herein, an asymmetric design of a Mo net/Li metal film (MLF) composite electrode is developed by an inverted thermal infusion method. The asymmetric MLF electrode has a dense oxide passivated layer on the top side, a porous Mo net matrix on the back side, and active Li layer in between. The back side has a larger specific area and higher electric field than the top side, which contacts with the separator upon cycling, triggering the preferred Li deposition and stripping of the porous back side of the electrode far from the separator. The surface passivation layer on the top side of the electrode as an artificial solid electrolyte interphase ensures the stable contact with the electrolyte and separator. Meanwhile, the porous structure of the supporting Mo net provides enough space for accommodating the volume change during Li deposition and stripping. This asymmetry design enables a unique “top down” growth pathway for Li deposition in the MLF electrode, suppressing the dendrite growth effectively. In conclusion, the design strategy provides a new direction for high-energy dendrite-free Li metal anodes.

25 ENERGY STORAGE↗

Surface Engineering of 3D Gas Diffusion Electrodes for High‐Performance H 2 Production with Nonprecious Metal Catalysts

Abstract In this work, a methodology is demonstrated to engineer gas diffusion electrodes for nonprecious metal catalysts. Highly active transition metal phosphides are prepared on carbon‐based gas diffusion electrodes with low catalyst loadings by modifying the O/C ratio at the surface of the electrode. These nonprecious metal catalysts yield extraordinary performance as measured by low overpotentials (51 mV at −10 mA cm −2 ), unprecedented mass activities (>800 A g −1 at 100 mV overpotential), high turnover frequencies (6.96 H 2 s −1 at 100 mV overpotential), and high durability for a precious metal‐free catalyst in acidic media. It is found that a high O/C ratio induces a more hydrophilic surface directly impacting the morphology of the CoP catalyst. The improved hydrophilicity, stemming from introduced oxyl groups on the carbon electrode, creates an electrode surface that yields a well‐distributed growth of cobalt electrodeposits and thus a well‐dispersed catalyst layer with high surface area upon phosphidation. This report demonstrates the high‐performance achievable by CoP at low loadings which facilitates further cost reduction, an important part of enabling the large‐scale commercialization of non‐platinum group metal catalysts. The fabrication strategies described herein offer a pathway to lower catalyst loading while achieving high efficiency and promising stability on a 3D electrode.

Sanchez, Joel↗

High-Speed Fabrication of Lithium-Ion Battery Electrodes by UV-Curing

In this study, UV-curing was investigated as an alternative method to provide fast production of composite cathodes and significantly reduce the time and energy required for solvent removal in lithium-ion battery fabrication. To serve our purpose, low-molecular-weight polysiloxane acrylate (PSA) was designed and synthesized from a polysiloxane epoxide precursor. In the presence of the acrylic acid additive LiNi1/ 3Mn1/3Co1/3O2 (NMC), electrode laminates containing 10 wt% PSA binder were successfully fabricated by UVcuring. The cured electrode exhibited good mechanical and electrochemical properties. At current rates up to C/3, the cell performance of the UV-cured NMC electrode was comparable to that of conventional polyvinylidene fluoride (PVDF)-bound NMC electrode. Our initial success in applying high-speed UV-curing in composite electrode fabrication has proved that it is a promising route to substantially reducing the capital and operation costs of lithium-ion battery electrode manufacturing and additionally bringing about important environmental benefits.

binder↗

Surface analysis insight note: X‐ray photoelectron spectroscopy analysis of battery electrodes—Challenges with nickel–manganese–cobalt and Li examples using an Al Kα x‐ray source

X‐ray photoelectron spectroscopy (XPS) has become a highly important tool for the analysis of battery materials and components. However, both anecdotal and detailed analysis of selected parts of the literature indicate that many reports of XPS on battery electrodes have significant analysis or data flaws. In this paper, we highlight several of the common challenges that analysts face when using XPS for battery materials, pointing to recent literature that addresses many of the critical issues associated with sample preparation as well as data collection and analysis. A common error for battery materials (and other materials) involves ignoring peak overlaps and interferences. Specifically, when a “minor” peak associated with a component in relatively high concentration overlaps or contributes to the primary peak (or one recommended for quantitative analysis) from a different element in the material. Overlap issues apply to many battery electrodes composed of many elements with complex photoelectron peak structures, as well as those involving peaks with seemingly simpler spectral envelopes such as Li and F. Examples of issues associated with battery systems are highlighted by a discussion of challenges associated with XPS analysis of Li and nickel–manganese–cobalt (NMC) electrodes in battery systems. Lithium analysis has challenges associated with the preparation and an often‐unrecognized peak overlap with F. In our laboratory and in the literature, NMC electrodes are often examined and new XPS users do not always recognize interference of the Auger signal from F KLL (in or on the electrode) with Ni 2p photoelectron spectrum when generated with Al Kα X‐rays. The use of simulated spectra involving both F and NiO demonstrates the extent of F Auger contributions to the Ni 2p signal strength as a function of the F/Ni atom ratio in the material and suggests spectra information that can be used to identify how significant effects will be on the resultant spectra. Our analysis demonstrates that in many cases overlap issues are significant for real electrode materials.

25 ENERGY STORAGE↗

Designing Low Tortuosity Electrodes through Pattern Optimization for Fast-Charging

The development of fast-charging technologies is crucial for expediting the progress and promotion of electric vehicles. In addition to innovative material exploration, reduction in the tortuosity of electrodes is a favored strategy to enhance the fast-charging capability of lithium-ion batteries by optimizing the ion-transfer kinetics. To realize the industrialization of low-tortuosity electrodes, a facile, cost-effective, highly controlled, and high-output continuous additive manufacturing roll-to-roll screen printing technology is proposed to render customized vertical channels within electrodes. Extremely precise vertical channels are fabricated by applying the as-developed inks, using LiNi 0.6 Mn 0.2 Co 0.2 O 2 as the cathode material. Additionally, the relationship between the electrochemical properties and architecture of the channels, including the pattern, channel diameter, and edge distance between channels, is revealed. The optimized screen-printed electrode exhibited a seven-fold higher charge capacity (72 mAh g -1 ) at a current rate of 6 C and superior stability compared with that of the conventional bar-coated electrode (10 mAh g -1 , 6 C) at a mass loading of 10 mg cm -2 . Finally, this roll-to-roll additive manufacturing can potentially be applied to various active materials printing to reduce electrode tortuosity and enable fast charging in battery manufacturing.

42 ENGINEERING↗

Representative volume element model of lithium-ion battery electrodes based on X-ray nano-tomography

For this, a new model that keeps all major advantages of the single-particle model of lithium-ion batteries (LIBs) and includes three-dimensional structure of the electrode was developed. Unlike the single spherical particle, this model considers a small volume element of an electrode, called the Representative Volume Element (RVE), which represent the real electrode structure. The advantages of using RVE as the model geometry was demonstrated for a typical LIB electrode consisting of nano-particle LiFePO 4 (LFP) active material. The three-dimensional morphology of the LFP electrode was reconstructed using a synchrotron X-ray nano-computed tomography at the Advanced Photon Source of the Argonne National. A 27 μm 3 cube from reconstructed structure was chosen as the RVE for the simulation purposes. The model was employed to predict the voltage curve in a half-cell during galvanostatic operations and validated with experimental data. The simulation results showed that the distribution of lithium inside the electrode microstructure is very different from the results obtained based on the single-particle model. The range of lithium concentration is found to be much greater, successfully illustrates the effect of microstructure heterogeneity.

25 ENERGY STORAGE↗