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DOE OSTI2020

A Comparative Study of Imidazolium-Based Ionic Liquid-Single-Walled Carbon Nanotube Composites with Enhanced Conductivity Properties for Supercapacitor Applications

Mixtures of ionic liquids (ILs) containing single-walled carbon nanotubes (SWCNTs) were prepared and characterized to obtain electrolytes with optimized transport properties for use in energy storage devices such as supercapacitors. Imidazolium ILs bearing cations with side chains of different functionality coupled with bis(trifluoromethylsulfonyl)amide (NTf 2- ) or bis(fluorosulfonyl)-amide (FSA-) anions, were used in mixtures containing up to 5 wt% SWCNTs. At and above 2 wt% nanotube loading, the mixtures exhibited higher conductivities than the pure ILs, in spite of the extremely high viscosities. Loadings of 5 wt% produced very high conductivities, and studies of the temperature dependence indicated a change in the charge transport mechanism between 2 and 5 wt% loading. At 5 wt% loading, the highest conductivities (up to 540 mS/cm at 25 °C) were obtained for the ILs containing the NTf 2- anion. Overall, these results can significantly contribute to the development of improved energy storage devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1996

Space Electrochemical Research and Technology

Individual papers presented at the conference address the following topics: development of a micro-fiber nickel electrode for nickel-hydrogen cell, high performance nickel electrodes for space power application, bending properties of nickel electrodes for nickel-hydrogen batteries, effect of KOH concentration and anions on the performance of a Ni-H2 battery positive plate, advanced dependent pressure vessel nickel hydrogen spacecraft cell and battery design, electrolyte management considerations in modern nickel hydrogen and nickel cadmium cell and battery design, a novel unitized regenerative proton exchange membrane fuel cell, fuel cell systems for first lunar outpost - reactant storage options, the TMI regenerable solid oxide fuel cell, engineering development program of a closed aluminum-oxygen semi-cell system for an unmanned underwater vehicle, SPE OBOGS on-board oxygen generating system, hermetically sealed aluminum electrolytic capacitor, sol-gel technology and advanced electrochemical energy storage materials, development of electrochemical supercapacitors for EMA applications, and high energy density electrolytic capacitor.

Richard M Wilson↗

NASA NTRS2017

Development of Structural Energy Storage for Aeronautics Applications

The National Aeronautics and Space Administration (NASA) has identified Multifunctional Structures for High Efficiency Lightweight Load-bearing Storage (M-SHELLS) as critical to development of hybrid gas-electric propulsion for commercial aeronautical transport in the N+3 timeframe. The established goals include reducing emissions by 80 and fuel consumption by 60 from todays state of the art. The advancement will enable technology for NASA Aeronautics Research Mission Directorates (ARMD) Strategic Thrust 3 to pioneer big leaps in efficiency and environmental performance for ultra-efficient commercial transports, as well as Strategic Thrust 4 to pioneer low-carbon propulsion technology in the transition to that scheme. The M-SHELLS concept addresses the hybrid gas-electric highest risk with its primary objective: to save structures energy storage system weight for future commercial hybrid electric propulsion aircraft by melding the load-carrying structure with energy storage in a single material. NASA's multifunctional approach also combines supercapacitor and battery chemistries in a synergistic energy storage arrangement in tandem with supporting good mechanical properties. The arrangement provides an advantageous combination of specific power, energy, and strength.

Santiago-Dejesus, Diana↗

DOE OSTI2021

Molecular Understanding of Charge Storage in MoS 2 Supercapacitors with Ionic Liquids

Owing to high electrical conductivity and ability to reversibly host a variety of inserted ions, 2D metallic molybdenum disulfide (1T-MoS 2 ) has demonstrated promising energy storage performance when used as a supercapacitor electrode. However, its charge storage mechanism is still not fully understood, in particular, how the interlayer spacing of 1T-MoS 2 would affect its capacitive performance. In this work, molecular dynamics simulations of 1T-MoS 2 with interlayer spacing ranging from 0.615 to 1.615 nm have been performed to investigate the resulting charge storage capacity in ionic liquids. Simulations reveal a camel-like capacitance-potential relation, and MoS 2 with an interlayer spacing of 1.115 nm has the highest volumetric and gravimetric capacitance of 118 F cm –3 and 42 F g –1 , respectively. Although ions in MoS 2 with an interlayer spacing of 1.115 nm diffuse much faster than with interlayer spacings of 1.365 and 1.615 nm, the MoS 2 with larger interlayer spacing has a much faster-charging process. Our analyses reveal that the ion number density and its charging speed, as well as ion motion paths, have significant impacts on the charging response. Here, this work helps to understand how the interlayer spacing affects the interlayer ion structures and the capacitive performance of MoS 2 , which is important for revealing the charge storage mechanism and designing MoS 2 supercapacitor.

25 ENERGY STORAGE↗

DOE OSTI2020

Bio-inspired redox mediated electrolyte for high performance flexible supercapacitor applications over broad temperature domain

For practical supercapacitors, recent advances in electrolytes have diminished long-standing problems such chemical stability, low ionic conductivity and limited electrochemical performance. Herewith, we communicate a facile method to produce anhydrous redox-active Bio-inspired electrolytes for flexible supercapacitors with application over a broad temperature range. The glycerol (Gly) gel electrolyte consists of various fractions of potassium hydroxide (KOH) and redox active unit, i.e., ammonium molybdate, (NH 4 ) 2 MoO 4 (abbreviated as Mo), in the anhydrous state. The doped glycerol matrix acts as a framework that provides a stable gel electrolyte, forming hierarchical pathway for ion diffusion. The developed gel network with Gly-KOH-MoX (X = 3, 5, 10, and 15%, w/w) provides an effective route to carry the ions onto the pores of the electrodes. The supercapacitor with Gly-KOH5-Mo10 gel provides a specific capacitance of 328 F g –1 , and the same device achieved an energy density of 45.6 Wh kg –1 at a power density of 497 W kg –1 . In addition, the supercapacitor maintained extraordinary cyclic robustness and wide temperature tolerance. Thus, the low cost and environmentally benign, cyclic durability of Gly-KOH-Mo makes these gel electrolytes a potential candidate for use in various energy storage devices.

25 ENERGY STORAGE↗

DOE OSTI2022

How do super concentrated electrolytes push the Li-ion batteries and supercapacitors beyond their thermodynamic and electrochemical limits?

Increasing the energy density of energy storage devices is currently the key target of many battery and supercapacitor research activities. For both types of devices, the electrochemical stability window (ESW) determines the effective energy density of the device. ESWs are defined by the effective oxidation and reduction potentials of the electrolyte, which are controlled by many various factors, including the HOMO/LUMO (highest/lowest unoccupied molecular orbital) energies of the electrolyte molecules, the nature of the electrode/electrolyte interphases, and other physicochemical properties. The concentration of the electrolyte would affect the HOMO/ LUMO levels thus also change the ESW. A higher concentration of salt induces specific arrangements among the anion, cation, and solvent molecules of an electrolyte, altering the bulk behavior of the electrolyte, resulting in drastic change in the electrode interfaces. These uniquely modified physicochemical properties extend the ESW in several different ways, including the enhancement in the kinetic stability of the electrodes, as well as the thermodynamic and Nernst shifts of the oxidation/reduction potentials of the electrolyte. For organic electrolytes, it is the reduced amount of free solvent molecules that plays the key role in such changes; whereas for aqueous electrolytes, it is the scarcity of free water molecules and the reduced water activity that control the key properties of the electrolyte. Here, we focus on elucidating the fundamental structural changes occurring within an electrolyte system with increasing salt concentrations. The underlying mechanisms which not only facilitates the extension of the ESW, but also enables higher rate capabilities and mitigates aluminum dissolution for batteries with organic electrolytes, are meticulously explained. Further, we thoroughly discuss the importance of high-voltage stability in aqueous battery systems by exploiting the changed properties observed with higher concentrations of salts. To finish, high-voltage supercapacitors enabled by superconcentrated electrolytes are also explored.

25 ENERGY STORAGE↗

DOE OSTI2021

Atomic/molecular layer deposition for energy storage and conversion

Energy storage and conversion systems, including batteries, supercapacitors, fuel cells, solar cells, and photoelectrochemical water splitting, have played vital roles in the reduction of fossil fuel usage, addressing environmental issues and the development of electric vehicles. The fabrication and surface/interface engineering of electrode materials with refined structures are indispensable for achieving optimal performances for the different energy-related devices. Atomic layer deposition (ALD) and molecular layer deposition (MLD) techniques, the gas-phase thin film deposition processes with self-limiting and saturated surface reactions, have emerged as powerful techniques for surface and interface engineering in energy-related devices due to their exceptional capability of precise thickness control, excellent uniformity and conformity, tunable composition and relatively low deposition temperature. In the past few decades, ALD and MLD have been intensively studied for energy storage and conversion applications with remarkable progress. In this work, we give a comprehensive summary of the development and achievements of ALD and MLD and their applications for energy storage and conversion, including batteries, supercapacitors, fuel cells, solar cells, and photoelectrochemical water splitting. Moreover, the fundamental understanding of the mechanisms involved in different devices will be deeply reviewed. Furthermore, the large-scale potential of ALD and MLD techniques is discussed and predicted. Finally, we will provide insightful perspectives on future directions for new material design by ALD and MLD and untapped opportunities in energy storage and conversion.

25 ENERGY STORAGE↗

DOE OSTI2020

Operando Tailoring of Defects and Strains in Corrugated β-Ni(OH) 2 Nanosheets for Stable and High-Rate Energy Storage

Nickel hydroxide represents a technologically important material for energy storage, such as hybrid supercapacitors. It has two different crystallographic polymorphs, α- and β-Ni(OH) 2 , showing advantages in either theoretical capacity or cycling/rate performance, manifesting a trade-off trend that needs to be optimized for practical applications. In this work, the synergistic superiorities in both activity and stability of corrugated β-Ni(OH) 2 nanosheets are demonstrated through an electrochemical abuse approach. With ≈91% capacity retention after 10 000 cycles, the corrugated β-Ni(OH) 2 nanosheets can deliver a gravimetric capacity of 457 C g -1 at a high current density of 30 A g -1 , which is nearly two and four times that of the regular α- and β-Ni(OH) 2 , respectively. Operando spectroscopy and finite element analysis reveal that greatly enhanced chemical activity and structural robustness can be attributed to the in situ tailored lattice defects and the strain-induced highly curved micromorphology. This work demonstrates a multi-scale defect-and-strain co-design strategy, which is helpful for rational design and tuned fabrication of next-generation electrode materials for stable and high-rate energy storage.

36 MATERIALS SCIENCE↗

DOE OSTI2021

USAID Grid-Scale Energy Storage Technologies Primer

This work provides an overview and compares key operating characteristics of select energy storage technologies. This work explores how these storage technologies may be used to improve the flexibility and reliability of power systems given their technical characteristics. The report covers various electrochemical (lithium-ion, lead-acid, flow, sodium-sulfur), chemical (hydrogen), mechanical (pumped hydro storage, compressed air energy storage, flywheels, gravity) and electrical (supercapacitors) storage mediums.

25 ENERGY STORAGE↗

DOE OSTI2022

An energy storage dispatch optimization for demand-side management in industrial facilities

An energy storage (ES) dispatch optimization was implemented to test lithium-ion battery ES, supercapacitor ES, and compressed air ES on two different industrial facilities – one intermittent process facility and one continuous process facility. The model first shows the capability of optimizing the size of a single technology on a single industrial facility to maximize the return on investment. Then, for the same profile, the model identifies significant differences in the optimal size for different technologies based on their performance parameters. Third, the model identifies differences in the optimal size for each technology based on the facilities profile. Here the results show compressed air ES yields the highest return on investment for both facilities and provides insight for future development of ES systems.

25 ENERGY STORAGE↗

DOE OSTI2021

Graphitized Biocarbon Derived from Hydrothermally Liquefied Low-Ash Corn Stover

Graphitized biocarbon can be utilized for energy storage applications such as supercapacitors. The scientific community have geared their attention to obtain such value-added product from abundantly available and low-cost biomass feedstock agricultural residues such as corn stover. Lignocellulosic components embedded within the cell wall of biomass substrates can provide a fine template for enhanced ion storage, transport, and rate capabilities, desirable for electrochemical storage. Presented is the utilization of homogenized low ash content corn stover milled and sieved to desired specifications, which underwent hydrothermal liquefaction in the presence of Ni-based catalytic salts at 275 o C. The hydrochar obtained by solid residue extracted from the reaction slurry was washed to acid neutral and subjected to catalytic activation using ZnCl 2 , followed by thermal annealing at 400 o C for morphological and pore size enhancement of the resulting biochar. Carbonization was performed on acid neutralized hydrochar at 850 °C to further enhance pore structures and increase graphitization for improved conductivity. Catalytic materials exhibited a specific capacitance of 316 F g -1 and held a 100% retention beyond 10,000 cycles. BET, Raman, XRD, cyclic voltammetry, chronopotentiometry, and EIS are discussed herein.

Biomass↗

DOE OSTI2023

Energy management systems for forecasted demand error compensation using hybrid energy storage system in nanogrid

This paper proposes an energy management system (EMS) for nanogrids to balance the power supply and forecasted demand in consideration of forecasting errors arising from high instantaneous demand. The proposed EMS employs a power-balancing optimization process for forecasted demand and a reference power modulation strategy for forecasting errors. This power-balancing optimization utilizes nanogrid sources, such as photovoltaics, fuel cells, and batteries, to meet forecasted demand and a supercapacitor charging process to overcome issues with a low energy density. The proposed reference power modulation strategy is utilized to allocate power from a hybrid energy storage system consisting of a battery and supercapacitor in order to compensate for forecasting errors. In addition, this proposed strategy considers battery and supercapacitor constraints such as the power changing rate and total power limitations. Further, the power-balancing optimization process also operates at faster sampling rate than the reference power modulation process in order to improve the computational efficiency. The performance of the proposed EMS is evaluated using real data obtained from the Korea Electric Power Exchange.

25 ENERGY STORAGE↗

DOE OSTI2022

In situ anodic electrodeposition of two-dimensional conductive metal-organic framework@nickel foam for high-performance flexible supercapacitor

Owing to their large specific surface area and well-defined porosity, metal-organic frameworks (MOFs) have long been considered as promising materials for energy storage. Unfortunately, their straightforward utilization in supercapacitors was hindered for years due to poor conductivity until the emergence of 2D conductive MOF materials. To date, several 2D conductive MOF-based supercapacitors have been reported. Nevertheless, almost all these supercapacitors were fabricated from MOF powders through a slurry coating method or dense packing method, which negatively affected their capacitor performance. Herein, we have developed an anodic electrodeposition (AED) approach to fabricate a uniformly deposited 2D conducting MOF on nickel foam and use it directly as electrodes for supercapacitors without any additives. Finally, the superior performance of the 2D conducting MOF on nickel foam in both aqueous and organic electrolytes was then disclosed by a series of electrochemical measurements, demonstrating the significant advantages of the AED approach over traditional methods.

2D conductive metal-organic frameworks↗

NASA NTRS2015

Assessment of Technologies for Noncryogenic Hybrid Electric Propulsion

The Subsonic Fixed Wing Project of NASA's Fundamental Aeronautics Program is researching aircraft propulsion technologies that will lower noise, emissions, and fuel burn. One promising technology is noncryogenic electric propulsion, which could be either hybrid electric propulsion or turboelectric propulsion. Reducing dependence on the turbine engine would certainly reduce emissions. However, the weight of the electricmotor- related components that would have to be added would adversely impact the benefits of the smaller turbine engine. Therefore, research needs to be done to improve component efficiencies and reduce component weights. This study projects technology improvements expected in the next 15 and 30 years, including motor-related technologies, power electronics, and energy-storage-related technologies. Motor efficiency and power density could be increased through the use of better conductors, insulators, magnets, bearings, structural materials, and thermal management. Energy storage could be accomplished through batteries, flywheels, or supercapacitors, all of which expect significant energy density growth over the next few decades. A first-order approximation of the cumulative effect of each technology improvement shows that motor power density could be improved from 3 hp/lb, the state of the art, to 8 hp/lb in 15 years and 16 hp/lb in 30 years.

Electric Propulsion↗

NASA NTRS2010

Low Mass Printable Devices for Energy Capture, Storage, and Use for Space Exploration Missions

The energy-efficient, environmentally friendly technology that will be presented is the result of a Space Act Agreement between -Technologies Worldwide, Inc., and the National Aeronautics and Space Administration s (NASA s) Marshall Space Flight Center (MSFC). This work combines semiconductor and printing technologies to advance lightweight electronic and photonic devices having excellent potential for commercial and exploration applications, and is an example of industry and government cooperation that leads to novel inventions. Device development involves three energy generation and consumption projects: 1) a low mass efficient (low power, low heat emission) micro light-emitting diode (LED) area lighting device; 2) a low-mass omni-directional efficient photovoltaic (PV) device with significantly improved energy capture; and 3) a new approach to building supercapacitors. These three technologies - energy capture, storage, and usage (e.g., lighting) - represent a systematic approach for building efficient local micro-grids that are commercially feasible; furthermore, these same technologies will be useful for lightweight power generation that enables inner planetary missions using smaller launch vehicles and facilitates surface operations. The PV device model is a two-sphere, light-trapped sheet approximately 2-mm thick. The model suggests a significant improvement over current thin film systems. All three components may be printed in line by printing sequential layers on a standard screen or flexographic direct impact press using the threedimensional printing technique (3DFM) patented by NthDegree. MSFC is testing the robustness of prototype devices in the harsh space and lunar surface environments, and available results will be reported. Unlike many traditional light sources, this device does not contain toxic compounds, and the LED component has passed stringent off-gassing tests required for potential manifesting on spacecraft such as the International Space Station. Future exploration missions will benefit from "green" technology lighting devices such as this, which show great promise for both terrestrial use and space missions.

Frazier, Donald O.↗

DOE OSTI2022

Surface engineering of MXenes for energy and environmental applications

We report MXenes, a new family of two-dimensional (2D) transition-metal carbides, nitrides, and carbonitrides, have received considerable attention in energy and environmental applications due to their intriguing electronic, electrochemical, optical, and chemical properties. Applications of MXenes have been witnessed in photocatalysis, electrocatalysis, thermocatalysis, sensing and biosensing, electrochemical energy storage, energy conversion and storage, rechargeable batteries, supercapacitors, and biomedicine. Notably, the tunable surface chemistry of MXenes plays an important role in their success in those applications. The surface composition of MXenes is considered to have a significant influence on their physicochemical properties and functionalities. In order to achieve a comprehensive understanding and rational design of MXenes by surface engineering, in this review, we highlight the application of several kinds of surface engineering approaches for MXenes, including tuning the surface termination groups, surface functionalization, surface defects, surface doping, surface oxidation, and the theoretical simulation of surface engineering of MXenes. Moreover, the relationship between the surface engineering and the physicochemical properties of MXenes is discussed. Finally, the ongoing challenges and opportunities for the future development of MXene surface engineering are also highlighted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Machine learning the electric field response of condensed phase systems using perturbed neural network potentials

Abstract The interaction of condensed phase systems with external electric fields is of major importance in a myriad of processes in nature and technology, ranging from the field-directed motion of cells (galvanotaxis), to geochemistry and the formation of ice phases on planets, to field-directed chemical catalysis and energy storage and conversion systems including supercapacitors, batteries and solar cells. Molecular simulation in the presence of electric fields would give important atomistic insight into these processes but applications of the most accurate methods such as ab-initio molecular dynamics (AIMD) are limited in scope by their computational expense. Here we introduce Perturbed Neural Network Potential Molecular Dynamics (PNNP MD) to push back the accessible time and length scales of such simulations. We demonstrate that important dielectric properties of liquid water including the field-induced relaxation dynamics, the dielectric constant and the field-dependent IR spectrum can be machine learned up to surprisingly high field strengths of about 0.2 V Å −1 without loss in accuracy when compared to ab-initio molecular dynamics. This is remarkable because, in contrast to most previous approaches, the two neural networks on which PNNP MD is based are exclusively trained on molecular configurations sampled from zero-field MD simulations, demonstrating that the networks not only interpolate but also reliably extrapolate the field response. PNNP MD is based on rigorous theory yet it is simple, general, modular, and systematically improvable allowing us to obtain atomistic insight into the interaction of a wide range of condensed phase systems with external electric fields.

Science & Technology - Other Topics↗

NASA NTRS2016

Influence of Molecular Simulation Model Accuracy on the Interfacial Properties of an Ionic Liquid: Overview of Recommended Practices

Increasing the energy storage capability of ionic liquid supercapacitors will require better understanding of ion-electrode interactions. We have probed the influence of these interactions on the structure and differential capacitance of of an ionic liquid ([EMIM][BF4]) at an ideal graphite interface as a function of model accuracy. Of note, differential capacitance is determined through newly derived and validated fluctuation formulas. In terms of model accuracy, we test electrostatic techniques, electrode charging techniques, and electrolyte interatomic potentials. For electrostatic summations, we employ high cost, high fidelity techniques as well as less expensive, approximate techniques for summation in slab geometry. For electrode charging, uniform, constant-charge and environmentally responsive, constant-potential conditions are employed. For the ionic liquid, constant charge and atomically polarizable models are employed. We comment on the role of model accuracy on the structure and energetics of the electric double layer as well as on the magnitude and shape of differential capacitance.

simulations↗