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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Oxygen-Vacancy Abundant Nanoporous Ni/NiMnO 3 /MnO 2 @NiMn Electrodes with Ultrahigh Capacitance and Energy Density for Supercapacitors

High-performance energy storage devices (HPEDs) play a critical role in the realization of clean energy and thus enable the overarching pursuit of nonpolluting, green technologies. Supercapacitors are one class of such lucrative HPEDs; however, a serious limiting factor of supercapacitor technology is its sub-par energy density. Here, this report presents hitherto unchartered pathway of physical deformation, chemical dealloying, and microstructure engineering to produce ultrahigh-capacitance, energy-dense NiMn alloy electrodes. The activated electrode delivered an ultrahigh specific-capacitance of 2700 F/cm 3 at 0.5 A/cm 3 . The symmetric device showcased an excellent energy density of 96.94 Wh/L and a remarkable cycle life of 95% retention after 10,000 cycles. Transmission electron microscopy and atom probe tomography studies revealed the evolution of a unique hierarchical microstructure comprising fine Ni/NiMnO 3 nanoligaments within MnO 2 -rich nanoflakes. Theoretical analysis using density functional theory showed semimetallic nature of the nanoscaled oxygen-vacancy-rich NiMnO 3 structure, highlighting enhanced carrier concentration and electronic conductivity of the active region. Furthermore, the geometrical model of NiMnO 3 crystals revealed relatively large voids, likely providing channels for the ion intercalation/de-intercalation. The current processing approach is highly adaptable and can be applied to a wide range of material systems for designing highly efficient electrodes for energy-storage devices.

25 ENERGY STORAGE↗
DOE OSTI2020

Understanding the Mechanism of High Capacitance in Nickel Hexaaminobenzene-Based Conductive Metal-Organic Frameworks in Aqueous Electrolytes

Recently, intrinsically conductive metal-organic frameworks (MOFs) have demonstrated promising performance in fast-charging energy storage applications and may outperform some current electrode materials (e.g., porous carbons) for supercapacitors in terms of both gravimetric and volumetric capacitance. In this report, we examine the mechanism of high capacitance in a nickel hexaaminobenzene-based MOF (NiHAB). Using a combination of in situ Raman and X-Ray absorption spectroscopies, as well as detailed electrochemical studies in a series of aqueous electrolytes, we demonstrate in this work that the charge storage mechanism is in fact a pH-dependent surface pseudocapacitance, and, unlike typical inorganic systems, where transition metals change oxidation state during charge/discharge cycles, NiHAB redox activity is ligand-centered.

25 ENERGY STORAGE↗
DOE OSTI2025

Energy-Efficient Capacitive Deionization through Electrode Modification and Process Development

Electrochemical separation technologies, such as capacitive deionization (CDI), are promising for addressing global energy and water challenges. However, there is a need to improve the performance, better understand property-performance relationships, and evaluate the longevity of CDI electrodes. This study explores the chemical modification of electrodes and the adjustment of CDI operating parameters. Results indicate that nitric acid (HNO3) conditioning of activated carbon cloth (ACC) electrodes removes metal oxides, introduces oxygen and nitrogen functionalities, and increases the specific capacitance (16% at 1 mV/s). Moreover, these changes in electrode properties positively impact device-level CDI performance. Through HNO3-conditioning of the ACC and tuning of the operational parameters, this work demonstrates higher electrosorption capacity (4.0x), greater charge efficiency (90% vs 24%), and lower energy consumption (3.8x). Despite these enhancements, limitations of the HNO 3 -conditioned ACC include decreased desorption kinetics and a 32% loss in electrosorption capacity after 200 cycles. Overall, this work provides guidance on using oxidative pretreatment via HNO 3 to modify ACC electrodes for CDI and evaluates the trade-offs associated with varying operational parameters.

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

Chemically Stable Polyarylether-Based Metallophthalocyanine Frameworks with High Carrier Mobilities for Capacitive Energy Storage

Covalent organic frameworks (COFs) with efficient charge transport and exceptional chemical stability are emerging as an import class of semiconducting materials for opto-/electronic devices and energy-related applications. However, the limited synthetic chemistry to access such materials and the lack of mechanistic understanding of carrier mobility greatly hinder their practical applications. Herein, we report the synthesis of three chemically stable polyarylether-based metallophthalocyanine COFs (PAE-PcM, M = Cu, Ni, and Co) and facile in situ growth of their thin films on various substrates (i.e., SiO 2 /Si, ITO, quartz) under solvothermal conditions. We show that PAE-PcM COFs thin films with van der Waals layered structures exhibit p -type semiconducting properties with the intrinsic mobility up to ~19.4 cm 2 V -1 s -1 and 4 orders of magnitude of increase in conductivity for PAE-PcCu film (0.2 S m -1 ) after iodine doping. Density functional theory calculations reveal that the carrier transport in the framework is anisotropic, with the out-of-plane hole transport along columnar stacked phthalocyanine more favorable. Furthermore, PAE-PcCo shows the redox behavior maximumly contributes ~88.5% of its capacitance performance, giving rise to a high surface area normalized capacitance of ~19 μF cm -2 . Overall, this work not only offers fundamental understandings of electronic properties of polyarylether-based 2D COFs but also paves the way for their energy-related applications.

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

Superior Capacitive Energy-Storage Performance in Pb-Free Relaxors with a Simple Chemical Composition

Chemical design of lead-free relaxors with simultaneously high energy density (W rec ) and high efficiency (η) for capacitive energy-storage has been a big challenge for advanced electronic systems. The current situation indicates that realizing such superior energy-storage properties requires highly complex chemical components. Herein, we demonstrate that, via local structure design, an ultrahigh W rec of 10.1 J/cm 3 , concurrent with a high η of 90%, as well as excellent thermal and frequency stabilities can be achieved in a relaxor with a very simple chemical composition. By introducing 6s 2 lone pair stereochemical active Bi into the classical BaTiO 3 ferroelectric to generate a mismatch between A- and B-site polar displacements, a relaxor state with strong local polar fluctuations can be formed. Through advanced atomic-resolution displacement mapping and 3D reconstructing the nanoscale structure from neutron/X-ray total scattering, it is revealed that the localized Bi enhances the polar length largely at several perovskite unit cells and disrupts the long-range coherent Ti polar displacements, resulting in a slush-like structure with extremely small size polar clusters and strong local polar fluctuations. This favorable relaxor state exhibits substantially enhanced polarization, and minimized hysteresis at a high breakdown strength. This work offers a feasible avenue to chemically design new relaxors with a simple composition for high-performance capacitive energy-storage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

A nanoporous capacitive electrochemical ratchet for continuous ion separations

Directed ion transport in liquid electrolyte solutions underlies many phenomena in natural and industrial settings. While nature has evolved structures that drive continuous ion flow without Faradaic redox reactions, establishing this process in synthetic systems has been challenging. Here, in this study, we report an ion pump that drives aqueous ions against a force using a capacitive ratchet mechanism independent of redox reactions. Modulation of an electric potential between thin metallic layers on either face of a nanoporous alumina wafer immersed in solution results in persistent voltages and ionic currents. This occurs due to the nonlinear capacitive nature of electric double layers, whose repeated charging and discharging sustains a continuous ion flux. Using this approach, we demonstrate ratchet-driven electrodialysis that reaches a 50% decrease in the conductivity of the solution in a dilution cell. These ratchet-based ion pumps can enable continuous desalination and selective ion separation using an electrically powered device with no moving parts.

Kautz, Rylan [University of California, Irvine, CA↗
DOE OSTI2012

Quantum Capacitance in Topological Insulators

Topological insulators show unique properties resulting from massless, Dirac-like surface states that are protected by time-reversal symmetry. Theory predicts that the surface states exhibit a quantum spin Hall effect with counter-propagating electrons carrying opposite spins in the absence of an external magnetic field. However, to date, the revelation of these states through conventional transport measurements remains a significant challenge owing to the predominance of bulk carriers. Here, we report on an experimental observation of Shubnikov-de Haas oscillations in quantum capacitance measurements, which originate from topological helical states. Unlike the traditional transport approach, the quantum capacitance measurements are remarkably alleviated from bulk interference at high excitation frequencies, thus enabling a distinction between the surface and bulk. We also demonstrate easy access to the surface states at relatively high temperatures up to 60 K. Our approach may eventually facilitate an exciting exploration of exotic topological properties at room temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Dielectric polymers for high-temperature capacitive energy storage

Polymers are the preferred materials for dielectrics in high-energy-density capacitors. The electrification of transport and growing demand for advanced electronics require polymer dielectrics capable of operating efficiently at high temperatures. In this review, we critically analyze the most recent development in the dielectric polymers for high-temperature capacitive energy storage applications. While general design considerations are discussed, emphasis is placed on the elucidation of the structural dependence of the high-field dielectric and electrical properties and the capacitive performance, including discharged energy density, charge–discharge efficiency and cyclability, of dielectric polymers at high temperatures. Here, advantages and limitations of current approaches to high-temperature dielectric polymers are summarized. Challenges along with future research opportunities are highlighted at the end of this article.

25 ENERGY STORAGE↗
DOE OSTI2021

Emerging investigator series: local pH effects on carbon oxidation in capacitive deionization architectures

In this work, the effect of pH and potential is examined for the oxidation of carbon cloth electrodes used in capacitive deionization (CDI) processes. The degree of oxidation of the electrode surface, examined using the electrode's potential of zero charge (E pzc ) and measured using chronoamperometry and cyclic voltammetry, is found to be strongly correlated to the pH of the solution at the interface. Local pH measurements are examined at anodes and cathodes in full CDI and membrane-assisted capacitive deionization (MCDI) cells at cell voltages ranging from 0.3–1.2 V. The cathode is shown to be basic under charging potentials while the anode is found to be acidic. This local pH is found to be highly transient during charging and discharging in CDI cells while the pH is found to be relatively static in the MCDI cells, maintaining a basic pH at the cathode and an acidic pH at the anode even when the cell is discharged. Ion exchange membranes (IEM) are found to have two functions: (1) limiting co-ion expulsion that results from specific ion adsorption and (2) limiting the effects of parasitic Faradaic reactions on the separation process by stabilizing the local pH thereby mitigating dissolved oxygen reduction at the cathode and lessening carbon oxidation at the anode. Performance comparisons including the salt adsorption capacity and charge efficiency are also compared for these systems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

Effect of adding small amount of inductive fields to O{sub 2}, Ar/O{sub 2} capacitively coupled plasmas

Electron energy distribution functions (EEDFs) of low pressure O{sub 2} plasma were measured by adding small amount of coil power in a capacitive discharge. When the plasma was generated by bias power only, the measured EEDF showed a bi-Maxwellian distribution. However, when a very small coil power (a few Watts) was added, the EEDF evolved abruptly into a Maxwellian distribution, while the electron density was decreased. In an Ar/O{sub 2} mixture discharge, this EEDF evolution to the Maxwellian was also observed at a relatively higher coil power. This abrupt change in EEDFs with a very small coil power appears to be attributed to a combined effect of collisionless heating by capacitive and induced electric fields.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2013

Simulation study of wave phenomena from the sheath region in single frequency capacitively coupled plasma discharges; field reversals and ion reflection

Capacitively coupled radio-frequency (RF) discharges have great significance for industrial applications. Collisionless electron heating in such discharges is important, and sometimes is the dominant mechanism. This heating is usually understood to originate in a stochastic interaction between electrons and the electric fields. However, other mechanisms may also be important. There is evidence of wave emission with a frequency near the electron plasma frequency, i.e., ω{sub pe}, from the sheath region in collisionless capacitive RF discharges. This is the result of a progressive breakdown of quasi-neutrality close to the electron sheath edge. These waves are damped in a few centimeters during their propagation from the sheath towards the bulk plasma. The damping occurs because of the Landau damping or some related mechanism. This research work reports that the emission of waves is associated with a field reversal during the expanding phase of the sheath. Trapping of electrons near to this field reversal region is observed. The amplitude of the wave increases with increasing RF current density amplitude J(tilde sign){sub 0} until some maximum is reached, beyond which the wave diminishes and a new regime appears. In this new regime, the density of the bulk plasma suddenly increases because of ion reflection, which occurs due to the presence of strong field reversal near sheath region. Our calculation shows that these waves are electron plasma waves. These phenomena occur under extreme conditions (i.e., higher J(tilde sign){sub 0} than in typical experiments) for sinusoidal current waveforms, but similar effects may occur with non-sinusoidal pulsed waveforms for conditions of experimental interest, because the rate of change of current is a relevant parameter. The effect of electron elastic collisions on plasma waves is also investigated.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2013

The influence of the secondary electron induced asymmetry on the electrical asymmetry effect in capacitively coupled plasmas

In geometrically symmetric capacitive radio-frequency plasmas driven by two consecutive harmonics, a dc self-bias can be generated as a function of the phase shift between the driving frequencies via the Electrical Asymmetry Effect (EAE). Recently, the Secondary Electron Asymmetry Effect (SEAE) was discovered (Lafleur et al., J. Phys. D: Appl. Phys. 46, 135201 (2013)): unequal secondary electron emission coefficients at both electrodes were found to induce an asymmetry in single-frequency capacitive plasmas. Here, we investigate the simultaneous presence of both effects, i.e., a dual-frequency plasma driven by two consecutive harmonics with different electrode materials. We find that the superposition of the EAE and the SEAE is generally non-linear, i.e., the asymmetries generated by each individual effect do not simply add up at all phases. The control ranges of the dc self-bias and the mean ion energy can be enlarged, if both effects are combined.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

Parallel double-plate capacitive proximity sensor modelling based on effective theory

A semi-analytical model for a double-plate capacitive proximity sensor is presented according to the effective theory. Three physical models are established to derive the final equation of the sensor. Measured data are used to determine the coefficients. The final equation is verified by using measured data. The average relative error of the calculated and the measured sensor capacitance is less than 7.5%. The equation can be used to provide guidance to engineering design of the proximity sensors.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Nanowire-based frequency-selective capacitive photodetector for resonant detection of infrared radiation at room temperature

Characteristics of a capacitive infrared photodetector that works at room temperature by registering a change in capacitance upon illumination are reported. If used in an ideal resonant inductor-resistor-capacitor circuit, it can exhibit zero dark current, zero standby power dissipation, infinite detectivity, and infinite light-to-dark contrast ratio. It is also made frequency-selective by employing semiconductor nanowires that selectively absorb photons of energies close to the nanowire's bandgap. Based on measured parameters, the normalized detectivity is estimated to be ∼3 × 10{sup 7} Jones for 1.6 μm IR wavelength at room temperature.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Electrical double layers and differential capacitance in molten salts from density functional theory

Classical density functional theory (DFT) is used to calculate the structure of the electrical double layer and the differential capacitance of model molten salts. The DFT is shown to give good qualitative agreement with Monte Carlo simulations in the molten salt regime. The DFT is then applied to three common molten salts, KCl, LiCl, and LiKCl, modeled as charged hard spheres near a planar charged surface. The DFT predicts strong layering of the ions near the surface, with the oscillatory density profiles extending to larger distances for larger electrostatic interactions resulting from either lower temperature or lower dielectric constant. In conclusion, overall the differential capacitance is found to be bell-shaped, in agreement with recent theories and simulations for ionic liquids and molten salts, but contrary to the results of the classical Gouy-Chapman theory.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Capacitated arc routing problem and its extensions in waste collection

Capacitated arc routing problem (CARP) is the youngest generation of graph theory that focuses on solving the edge/arc routing for optimality. Since many years, operational research devoted to CARP counterpart, known as vehicle routing problem (VRP), which does not fit to several real cases such like waste collection problem and road maintenance. In this paper, we highlighted several extensions of capacitated arc routing problem (CARP) that represents the real-life problem of vehicle operation in waste collection. By purpose, CARP is designed to find a set of routes for vehicles that satisfies all pre-setting constraints in such that all vehicles must start and end at a depot, service a set of demands on edges (or arcs) exactly once without exceeding the capacity, thus the total fleet cost is minimized. We also addressed the differentiation between CARP and VRP in waste collection. Several issues have been discussed including stochastic demands and time window problems in order to show the complexity and importance of CARP in the related industry. A mathematical model of CARP and its new version is presented by considering several factors such like delivery cost, lateness penalty and delivery time.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

On the self-excitation mechanisms of plasma series resonance oscillations in single- and multi-frequency capacitive discharges

The self-excitation of plasma series resonance (PSR) oscillations is a prominent feature in the current of low pressure capacitive radio frequency discharges. This resonance leads to high frequency oscillations of the charge in the sheaths and enhances electron heating. Up to now, the phenomenon has only been observed in asymmetric discharges. There, the nonlinearity in the voltage balance, which is necessary for the self-excitation of resonance oscillations with frequencies above the applied frequencies, is caused predominantly by the quadratic contribution to the charge-voltage relation of the plasma sheaths. Using Particle In Cell/Monte Carlo collision simulations of single- and multi-frequency capacitive discharges and an equivalent circuit model, we demonstrate that other mechanisms, such as a cubic contribution to the charge-voltage relation of the plasma sheaths and the time dependent bulk electron plasma frequency, can cause the self-excitation of PSR oscillations, as well. These mechanisms have been neglected in previous models, but are important for the theoretical description of the current in symmetric or weakly asymmetric discharges.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Enhancement of two dimensional electron gas concentrations due to Si{sub 3}N{sub 4} passivation on Al{sub 0.3}Ga{sub 0.7}N/GaN heterostructure: strain and interface capacitance analysis

Enhancement of two dimensional electron gas (2DEG) concentrations at Al{sub 0.3}Ga{sub 0.7}N/GaN hetero interface after a-Si{sub 3}N{sub 4} (SiN) passivation has been investigated from non-destructive High Resolution X-ray Diffraction (HRXRD) analysis, depletion depth and capacitance-voltage (C-V) profile measurement. The crystalline quality and strained in-plane lattice parameters of Al{sub 0.3}Ga{sub 0.7}N and GaN were evaluated from double axis (002) symmetric (ω-2θ) diffraction scan and double axis (105) asymmetric reciprocal space mapping (DA RSM) which revealed that the tensile strain of the Al{sub 0.3}Ga{sub 0.7}N layer increased by 15.6% after SiN passivation. In accordance with the predictions from theoretical solution of Schrödinger-Poisson’s equations, both electrochemical capacitance voltage (ECV) depletion depth profile and C-V characteristics analyses were performed which implied effective 9.5% increase in 2DEG carrier density after passivation. The enhancement of polarization charges results from increased tensile strain in the Al{sub 0.3}Ga{sub 0.7}N layer and also due to the decreased surface states at the interface of SiN/Al{sub 0.3}Ga{sub 0.7}N layer, effectively improving the carrier confinement at the interface.

36 MATERIALS SCIENCE↗