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DOE OSTI2024

Electrochemical Capacitance Traces with Interlayer Spacing in Two‐dimensional Conductive Metal–Organic Frameworks

Abstract Electrically conductive metal–organic frameworks (MOFs) are promising candidates for electrochemical capacitors (EC) for fast energy storage due to their high specific surface areas and potential for redox activity. To maximize energy density, traditional inorganic pseudocapacitors have utilized faradaic processes in addition to double‐layer capacitance. Although conductive MOFs are usually comprised of redox active ligands which allow faradaic reactions upon electrochemical polarization, systematic studies providing deeper understanding of the charge storage processes and structure‐function relationships have been scarce. Here, we investigate the charge storage mechanisms of a series of triazatruxene‐based 2D layered conductive MOFs with variable alkyl functional groups, Ni 3 (HIR 3 ‐TAT) 2 (TAT=triazatruxene; R=H, Et, n ‐Bu, n ‐Pent). Functionalization of the triazatruxene core allows for systematic variation of structural parameters while maintaining in‐plane conjugation between ligands and metals. Specifically, R groups modulate interlayer spacing, which in turn shifts the charge storage mechanism from double‐layer capacitance towards pseudocapacitance, leading to an increase in molar specific capacitance from Ni 3 (HIH 3 ‐TAT) 2 to Ni 3 (HIBu 3 ‐TAT) 2 . Partial exfoliation of Ni 3 (HIBu 3 ‐TAT) 2 renders redox active ligand moieties more accessible, and thus increases the dominance of faradaic processes. Our strategy of controlling charge storage mechanism through tuning the accessibility of redox‐active sites may motivate further design and engineering of electrode materials for EC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Structural metamaterials with innate capacitive and resistive sensing

Interpenetrating lattices consist of two or more interwoven but physically separate sub-lattices with unique behaviors derived from their multi-body construction. If the sublattices are constructed or coated with an electrically conducting material, the close proximity and high surface area of the electrically isolated conductors allow the two lattices to interact electromagnetically either across the initial dielectric filled gap or through physical contact. Furthermore, changes in the size of the dielectric gap between the sub-lattices induced by deformation can be measured via capacitance or resistance, allowing a structurally competent lattice to operate as a force or deformation sensor. In addition to resistive and capacitive deformation sensing, this work explores capacitance as a fundamental metamaterial property and the environmental sensing behaviors of interpenetrating lattices.

Computational Solid Mechanics↗

DOE OSTI2019

Carbon polyaniline capacitive deionization electrodes with stable cycle life

Electrode materials for capacitive deionization (CDI), an energy efficient method for desalination, were developed in this work. Waste-tire derived carbon (TC) coated with polyaniline was used to form a carbon polymer composite (CPC). CPC was used as an electrode in CDI configurations to determine the salt adsorption capability of the material. Chemical treatment of TC with KOH led to an enhancement in surface area to 952 m 2 /g and microporosity in the sub-2-nm range. This unique microstructure is considered to be beneficial for effective ion uptake in CDI applications. The capacitance of the electrodes was further enhanced through surface coating with polyaniline, resulting in a specific capacitance of 168.2 F/g. In batch cell testing with 1.2 V applied potential, the salt adsorption capacity (SAC), measured in mg of salt adsorbed per gram of active material, in a 1500–1700 ppm KCl solution was measured at 14.2 mg/g. Scale-up of the process with ionic-membrane-assisted CDI (MCDI) led to improvement in SAC at 18.9 mg/g. Further, cycling tests revealed that the electrodes had comparable or better longevity compared to other CDI materials, retaining >92.8% charging capacity after 300 cycles. In conclusion, high adsorption capacities for other salts such as LiCl, NaCl, MgCl 2 and CaCl 2 have been found.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Capacitance of Ti 3 C 2 T x MXene in Ionic Liquid Electrolyte

Ti 3 C 2 T x MXene, a two-dimensional (2D) early transition metal carbide, has shown an extremely high volumetric capacitance in aqueous electrolytes, but in a narrow voltage window (less than 1.23 V). The utilization of MXene materials in ionic liquid electrolytes with a large voltage window has never been addressed. Here, we report the preparation of the Ti 3 C 2 T x MXene ionogel film by vacuum filtration for use as supercapacitor electrodes operating in 1-Ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMI-TFSI) neat ionic liquid electrolyte. Due to the disordered structure of the Ti 3 C 2 T x hydrogel film and a stable spacing after vacuum drying, achieved through ionic liquid electrolyte immersion of the Ti 3 C 2 T x hydrogel film, the Ti 3 C 2 T x surface became accessible to EMI + and TFSI - ions. A capacitance of 70 F g -1 together with a large voltage window of 3 V was obtained at a scan rate of 20 mV s -1 in neat EMI-TFSI electrolyte. The electrochemical signature indicates a capacitive behavior even at a high scan rate (500 mV s -1 ) and a high power performance. This work opens up the possibilities of using MXene materials with various ionic liquid electrolytes.

25 ENERGY STORAGE↗

DOE OSTI2014

Capacitance and conductance characterization of nano-ZnGa{sub 2}Te{sub 4}/n-Si diode

Graphical abstract: - Highlights: • XRD and DTA micrographs were used to study the structure of ZnGa{sub 2}Te{sub 4}. • C–V, G–V and R{sub s}–V of the diode characteristics have been analyzed for the first time. • Dielectric constant, dielectric loss, loss tangent and ac conductivity were determined. • The interfaces states were determined using conductance–voltage technique. • ZnGa{sub 2}Te{sub 4} is a good candidate for electronic device applications. - Abstract: Capacitance–voltage (C–V) and conductance–voltage (G–V) characteristics of p-ZnGa{sub 2}Te{sub 4}/n-Si HJD were studied over a wide frequency and temperature. Both the interface states density N{sub ss} and series resistance R{sub s} were strongly frequency and temperature dependent. The interface states density N{sub ss} is decreased with increasing frequency and increase with increasing temperature. The values of the built-in potential (V{sub bi}) were calculated and found to increase with increasing temperature and frequency. The values of capacitance C, conductance G, series resistance R{sub s}, corrected capacitance C{sub ADJ}, corrected conductance G{sub ADJ}, dielectric constant (ε′), dielectric loss (ε″), loss tangent (tan δ) and the AC conductivity (σ{sub ac}) are strongly dependent on the applied frequency, voltage and temperature. The obtained results show that the locations of N{sub ss} and R{sub s} have a significant effect on the electrical characteristics of the studied diode.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Synthesis of porous MnO2-CoO microsheets and nanocones as a high-performance battery-type capacitive material

Highlights: • Porous MnO{sub 2}-CoO microsheets and nanocones (MCMSNCs) are synthesized. • Sodium dodecyl sulfate controls the formation of specific metal oxide structures. • MCMSNCs deliver excellent capacitive performance as a battery-type material. - Abstract: A facile method via sodium dodecyl sulfate (SDS)-templated oil-bath followed by annealing treatment is reported to synthesize porous MnO{sub 2}-CoO microsheets and nanocones (MCMSNCs). Herein, surfactant SDS is firstly used to obtain Mn/Co hydroxide ultrathin microsheets and nanocones precursor, which is then transformed into interconnected porous MCMSNCs after heat treatment. As a battery-type capacitive electrode micro/nanomaterial, MCMSNCs exhibit an original specific capacity (148 C g{sup −1}) at a current density of 1 A g{sup −1} by chronopotentiometry. Moreover, MCMSNCs deliver good rate performance with 77% capacity retention from 1 to 16 A g{sup −1} and excellent cycle life with 20% loss of the maximum value as well as 118% retention of the initial one after 3000 cycles. The excellent capacitive performance of porous MCMSNCs endows it potential use as an anode electrode material in the application of electrochemical capacitors.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2016

Reduced graphene oxide hydrogels deposited in nickel foam for supercapacitor applications: Toward high volumetric capacitance

Graphene hydrogels have been considered as ideal materials for high-performance supercapacitors. However, their low volumetric capacitance significantly limits its real application. In this study, we report an environment-friendly and scalable method to prepare high packing density, electrochemically reduced graphene oxide hydrogels (ERGO) for supercapacitor application by the electrophoretic deposition of graphene oxide onto nickel foam, followed by the electrochemical reduction and hydraulic compression of the deposited materials. The as-prepared ERGO on nickel foam was hydraulic compressed up to 20 tons, resulting in an increase of the packing density of ERGO from 0.0098 to 1.32 g cm –3 . Consequently, the volumetric capacitance and volumetric energy density of ERGOs greatly increased from 1.58 F cm –3 and 0.053 Wh cm –3 (as-prepared ERGO) to 176.5 F cm –3 and 6.02 Wh cm –3 (ERGO compressed at 20 tons), respectively. The ERGOs also exhibited long-term electrochemical stability with a capacitance retention in the range of approximately 79–90% after 10 000 cycles. Lastly, we believe that these high packing density ERGOs are promising for real-world energy storage devices for which scalable, cost-effective manufacturing is of significance and for which space constraints are paramount.

25 ENERGY STORAGE↗

DOE OSTI2019

Dynamical nonlinear memory capacitance in biomimetic membranes

Two-terminal memory elements, or memelements, capable of co-locating signal processing and memory via history-dependent reconfigurability at the nanoscale are vital for next-generation computing materials striving to match the brain’s efficiency and flexible cognitive capabilities. While memory resistors, or memristors, have been widely reported, other types of memelements remain underexplored or undiscovered. Here we report the first example of a volatile, voltage-controlled memcapacitor in which capacitive memory arises from reversible and hysteretic geometrical changes in a lipid bilayer that mimics the composition and structure of biomembranes. We demonstrate that the nonlinear dynamics and memory are governed by two implicitly-coupled, voltage-dependent state variables—membrane radius and thickness. Further, our system is capable of tuneable signal processing and learning via synapse-like, short-term capacitive plasticity. These findings will accelerate the development of low-energy, biomolecular neuromorphic memelements, which, in turn, could also serve as models to study capacitive memory and signal processing in neuronal membranes.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Understanding resistances in capacitive deionization devices

The desalination characteristics of capacitive deionization (CDI) are significantly impacted by the cell resistance. Here we apply electrochemical impedance spectroscopy (EIS) to analyze the resistive properties of a CDI device, which include EIS measurements on a complete assembled cell (in two wire mode) and EIS measurements with additional contacts to decouple electrode/electrolyte and contact impedances (four wire mode). These measurements shed light on the interface between current collector and electrode as well as the internal capacitive and resistive elements of the cell. With two-wire and four-wire EIS measurements, we find that the often observed high-frequency arc(s) in the impedance spectra can be due to contact effects and/or an internal ionic-transfer resistance that is locally in parallel with macropore wall capacitance. In some cases, the two associated arcs in the Nyquist plot are overlapping and present simultaneously, making their identification in the EIS spectra difficult unless both two-wire and four-wire measurements are made. Despite causing a large high-frequency arc in the Nyquist plot, we find that the apparent internal ionic-transfer resistance is negligible compared to the resistances of the electrode, separator, and external electronic components. Here, an investigation of the contact impedance between the electrode and current collector reveals a parallel RC arc that can grow over time if an improper material is used (e.g., titanium). In our system, the electrode ionic resistance dominates the total Ohmic power dissipation, which has implications for scale-up of CDI systems and future improvements of cell design.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Sensitivity map computation in adaptive electrical capacitance volume tomography with multielectrode excitations

Electrical capacitance tomography (ECT) is a low‐cost, high‐speed imaging technique useful in many industrial settings. ECT is predicated on the knowledge of sensitivity maps between capacitance electrodes that blanket the imaging domain. The simultaneous activation of multiple electrodes can be advantageous to manipulate the resulting field distributions and capture additional spatial information for imaging purposes. However, conventional methods for sensitivity map computation in ECT are not adequate in the presence of multielectrode activation because the mutual coupling between electrodes is not properly accounted for. This coupling becomes especially critical in adaptive electrical capacitance volume tomography (AECVT) sensors, where signals from many small electrode segments are combined into synthetic electrodes. A more general approach is presented for sensitivity map computation in AECVT based on the actual posteriori (induced) charge distributions rather than the conventional approach based on boundary conditions with no account for electrode interactions.

Zeeshan, Z.↗

DOE OSTI2011

Measurements of time average series resonance effect in capacitively coupled radio frequency discharge plasma

Self-excited plasma series resonance is observed in low pressure capacitvely coupled radio frequency discharges as high-frequency oscillations superimposed on the normal radio frequency current. This high-frequency contribution to the radio frequency current is generated by a series resonance between the capacitive sheath and the inductive and resistive bulk plasma. In this report, we present an experimental method to measure the plasma series resonance in a capacitively coupled radio frequency argon plasma by modifying the homogeneous discharge model. The homogeneous discharge model is modified by introducing a correction factor to the plasma resistance. Plasma parameters are also calculated by considering the plasma series resonances effect. Experimental measurements show that the self-excitation of the plasma series resonance, which arises in capacitive discharge due to the nonlinear interaction of plasma bulk and sheath, significantly enhances both the Ohmic and stochastic heating. The experimentally measured total dissipation, which is the sum of the Ohmic and stochastic heating, is found to increase significantly with decreasing pressure.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2013

Capacitance enhancement via electrode patterning

The necessity of increasing the energy density in electric double layer capacitors to meet current demand is fueling fundamental and applied research alike. We report here molecular dynamics simulation results for aqueous electrolytes near model electrodes. Particular focus is on the effect of electrode patterning on the structure of interfacial electrolytes, and on the potential drop between the solid electrodes and the bulk electrolytes. The latter is estimated by numerically integrating the Poisson equation using the charge densities due to water and ions accumulated near the interface as input. We considered uniform and patterned electrodes, both positively and negatively charged. The uniformly charged electrodes are modeled as graphite. The patterned ones are obtained by removing carbon atoms from the top-most graphene layer, yielding nanoscopic squares and stripes patterns. For simplicity, the patterned electrodes are effectively simulated as insulators (the charge remains localized on the top-most layer of carbon atoms). Our simulations show that the patterns alter the structure of water and the accumulation of ions at the liquid-solid interfaces. Using aqueous NaCl solutions, we found that while the capacitance calculated for three positively charged electrodes did not change much, that calculated for the negatively charged electrodes significantly increased upon patterning. We find that both water structure and orientation, as well as ion accumulation affect the capacitance. As electrode patterning affects differently water structure and ion accumulation, it might be possible to observe ion-specific effects. These results could be useful for advancing our understanding of electric double layer capacitors, capacitive desalination processes, as well as of fundamental interfacial electrolytes properties.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Capacitive energy storage and recovery for synchrotron magnets

Feasibility studies on capacitive energy storage and recovery in the main-ring synchrotron of the Japan Proton Accelerator Research Complex were conducted by circuit simulation. The estimated load fluctuation was 96 MVA in total for dipole magnets, which is likely to induce a serious disturbance in the main grid. It was found that the energy stored in the magnets after the excitation period can be recovered to the storage capacitor by controlling the voltage across the energy-storage capacitor using a pulse-width-modulation converter and reused in the next operational cycle. It was also found that the power fluctuation in the main grid can be reduced to 12 MVA. An experimental evaluation of an aluminum metalized film capacitor revealed that capacitance loss was induced by a fluctuating voltage applied to the storage capacitor when applying the proposed method. The capacitance loss was induced by corona discharge around the edges of segmented electrodes of a self-healing capacitor. The use of aluminum-zinc alloy was evaluated as a countermeasure to mitigate the effect induced by the corona discharge. For a zinc content of 8%, which was optimized experimentally, a capacitor with a sufficient life time expectancy of 20 years and a working potential gradient of 250 V/μm was developed.

43 PARTICLE ACCELERATORS↗

DOE OSTI2016

Optical characteristics for capacitively and inductively radio frequency discharge and post-discharge of helium

The optical properties for radiofrequency (RF) post-discharge of pure helium (He) with two different methods as capacitively and inductively have been presented using the modified Boltzmann method in comparison. Optical emission spectroscopy (OES) is often used in the diagnosis of laboratory plasma, such as gas discharge plasma. OES is a very useful method for calculating of the electron temperature in the plasma and the determination of different atoms and molecules. In this study, OES is applied for characterizations of capacitively and inductively RF He plasma at pressures between 0.62 and 2.2 mbar for newly reactor type. Plasmas are generated with an RF power generator at a frequency of 13.56 MHz and output powers of 100, 160, and 200 W. Spectra have been evaluated in the range 200–1200 nm by an optical spectrometer. At low pressure, the main spectral features reported are the wavelengths of the atomic He transitions at 388.87 and 728.13 nm. The atomic emission intensities showed a maximum in inductive system when the pressure is about 0.62 mbar. OES of capacitive discharge and inductive discharge is compared in detail. The transition for 587.56 nm is shown to be increased in time.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2016

Material characteristics and equivalent circuit models of stacked graphene oxide for capacitive humidity sensors

The oxidation properties of graphene oxide (GO) are systematically correlated with their chemical sensing properties. Based on an impedance analysis, the equivalent circuit models of the capacitive sensors are established, and it is demonstrated that capacitive operations are related to the degree of oxidation. This is also confirmed by X-ray diffraction and Raman analysis. Finally, highly sensitive stacked GO sensors are shown to detect humidity in capacitive mode, which can be useful in various applications requiring low power consumption.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2018

Electrodynamics of ferroelectric films with negative capacitance

We construct a theory of the electrodynamic response of ferroelectric thin films containing periodic domain textures (PDTs) with 180° polarization-oriented domains. Here, we demonstrate that a depolarization field induced by PDTs gives rise to the negative capacitance of the ferroelectric film. We derive frequency-dependent dielectric permittivity related to the PDT dynamics across the entire frequency range. We find the resonance mode of domain oscillations in the terahertz (THz) spectral band and the singular points in the phase of the reflected THz beam that are intimately related to the negative capacitance. Our findings provide a material platform for the THz negative-capacitance-based optics of ferroelectric films and for epsilon-near-zero plasmonic THz metamaterials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Capacitive response of biological membranes

We present a minimal model to analyze the capacitive response of a biological membrane subjected to a step voltage via blocking electrodes. Through a perturbative analysis of the underlying electrolyte transport equations, we show that the leading-order relaxation of the transmembrane potential is governed by a capacitive timescale, τ_{C}=λ_{D}L/D(2+Γδ^{M}/L/4+Γδ^{M}/λ_{D}), where λ_{D} is the Debye screening length, L is the electrolyte width, Γ is the ratio of the permittivity of the electrolyte to the membrane, δ^{M} is the membrane thickness, and D is the ionic diffusivity. This timescale is considerably shorter than the traditional RC timescale λ_{D}L/D for a bare electrolyte due to the membrane's low permittivity and finite thickness. Beyond the linear regime, however, salt diffusion in the bulk electrolyte drives a secondary, nonlinear relaxation process of the transmembrane potential over a longer timescale τ_{L}=L^{2}/4π^{2}D. A simple equivalent-circuit model accurately captures the linear behavior, and the perturbation expansion remains applicable across the entire range of observed physiological transmembrane potentials. Together, these findings underscore the importance of the faster capacitive timescale and nonlinear effects on the bulk diffusion timescale in determining transmembrane potential dynamics for a range of biological systems.

Farhadi, Jafar↗

DOE OSTI2021

Comparison of the Capacitances and Switching Losses of 1.2 kV Common-Source and Common- Drain Bidirectional Switch Topologies

Bidirectional, or four-quadrant switches (FQS) can be designed as back-to-back MOSFETs connected in common-drain (CD) or common-source (CS) topologies. CDFQS and CS-FQS assembled from discrete 1.2 kV commercially available SiC power MOSFETs were characterized to obtain capacitance and switching loss values. The CD-FQS exhibited a 1.17x larger turn-on loss compared to the CS-FQS, while the CS-FQS exhibited a 1.52x larger turn-off loss compared to the CD-FQS. The CS-FQS exhibited a lower input capacitance, while the CD-FQS exhibited a lower output and reverse transfer capacitance.

Silicon Carbide, Bidirectional Switch, Switching P↗