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At least 271 records · Page 15

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DOE OSTI2024

Enhancing the dark-state bistability and thermal stability of zinc dynamic windows with nitrile electrolytes

Reversible metal electrodeposition (RME) for dynamic windows is a promising alternative to traditional electrochromics. We explore the reasons behind the bistability of practical RME dynamic windows under a wide temperature range, i.e., how well they maintain their dark state without external power. While Zn dynamic windows with dimethyl sulfoxide electrolytes exhibit adequate bistability at room temperature, their performance degrades at elevated temperatures due to the presence of small amounts of water. Here, to overcome this problem, we developed a set of Zn nitrile electrolytes. The integrated devices can maintain dark-state bistability over at least 1 month at 85°C with 0.1% transmission using a propionitrile (PrCN) electrolyte. Additionally, the PrCN-based Zn dynamic windows possess high optical contrast, color-neutral switching, and promising cyclability, making Zn RME in nitrile electrolytes a promising solution for achieving robust dynamic windows.

RME↗

NASA NTRS1993

High power density proton exchange membrane fuel cells

Proton exchange membrane (PEM) fuel cells use a perfluorosulfonic acid solid polymer film as an electrolyte which simplifies water and electrolyte management. Their thin electrolyte layers give efficient systems of low weight, and their materials of construction show extremely long laboratory lifetimes. Their high reliability and their suitability for use in a microgravity environment makes them particularly attractive as a substitute for batteries in satellites utilizing high-power, high energy-density electrochemical energy storage systems. In this investigation, the Dow experimental PEM (XUS-13204.10) and unsupported high platinum loading electrodes yielded very high power densities, of the order of 2.5 W cm(exp -2). A platinum black loading of 5 mg per cm(exp 2) was found to be optimum. On extending the three-dimensional reaction zone of fuel cell electrodes by impregnating solid polymer electrolyte into the electrode structures, Nafion was found to give better performance than the Dow experimental PEM. The depth of penetration of the solid polymer electrolyte into electrode structures was 50-70 percent of the thickness of the platinum-catalyzed active layer. However, the degree of platinum utilization was only 16.6 percent and the roughness factor of a typical electrode was 274.

Murphy, Oliver J.↗

NASA NTRS2010

Supercapacitor Electrolyte Solvents with Liquid Range Below -80 C

A previous NASA Tech Brief ["Low-Temperature Supercapacitors" (NPO-44386) NASA Tech Briefs, Vol. 32, No 7 (July 2008), page 32] detailed ongoing efforts to develop non-aqueous supercapacitor electrolytes capable of supporting operation at temperatures below commercially available cells (which are typically limited to charging and discharging at > or equal to -40 C). These electrolyte systems may enable energy storage and power delivery for systems operating in extreme environments, such as those encountered in the Polar regions on Earth or in the exploration of space. Supercapacitors using these electrolytes may also offer improved power delivery performance at moderately low temperatures (e.g. -40 to 0 C) relative to currently available cells, offering improved cold-cranking and cold-weather acceleration capabilities for electrical or hybrid vehicles. Supercapacitors store charge at the electrochemical double-layer, formed at the interface between a high surface area electrode material and a liquid electrolyte. The current approach to extending the low-temperature limit of the electrolyte focuses on using binary solvent systems comprising a high-dielectric-constant component (such as acetonitrile) in conjunction with a low-melting-point co-solvent (such as organic formates, esters, and ethers) to depress the freezing point of the system, while maintaining sufficient solubility of the salt. Recent efforts in this area have led to the identification of an electrolyte solvent formulation with a freezing point of -85.7 C, which is achieved by using a 1:1 by volume ratio of acetonitrile to 1,3-dioxolane

Brandon, Erik↗

NASA NTRS1984

Factors Affecting Nickel-oxide Electrode Capacity in Nickel-hydrogen Cells

The nickel-oxide electrode common to the nickel hydrogen and nickel cadmium cell is by design the limiting or capacity determining electrode on both charge and discharge. The useable discharge capacity from this electrode, and since it is the limiting electrode, the useable discharge capacity of the cell as well, can and is optimized by rate of charge, charge temperature and additives to electrode and electrolyte. Recent tests with nickel hydrogen cells and tests performed almost 25 years ago with nickel cadmium cells indicate an improvement of capacity as a result of using increased electrolyte concentration.

Ritterman, P. F.↗

DOE OSTI2025

Impact of Electrolyte Solvent on Li 4 Ti 5 O 12 /LiNi 0.90 Mn 0.05 Co 0.05 O 2 Battery Performance for Behind-the-Meter Storage Applications

Behind-the-Meter Storage (BTMS) systems require dedicated development of battery materials that target long cycle life and low cost at the system level. Pairing Li 4 Ti 5 O 12 (LTO) and LiNi 0.9 Mn 0.05 Co 0.05 O 2 (NMC90-5-5) shows promise to achieve targets for BTMS applications; however, minimal literature is available that discusses electrolyte solvent selection for this pairing. This study explores the role of electrolyte solvent on cycle life in LTO/NMC90-5-5 batteries. Four model electrolytes are evaluated; the baseline, Gen2, is compared with 1M LiPF 6 added to each of three separate solvents: ethylene carbonate (EC), ethyl methyl carbonate (EMC), and fluoroethylene carbonate (FEC). An additional consideration is that NMC90-5-5 undergoes an H2→H3 phase transition that allows for a significant increase to capacity; however, it’s unclear how this phase transition impacts electrolyte stability and cycle life. Therefore, the phase transition is avoided or accessed by cycling to 2.6V or 2.7V, respectively. The cells with Gen2, cycled to 2.6V, show the highest capacity retention due to EC passivating the LTO, EMC improving stability at the NMC90-5-5, and avoiding increased degradation from the 2.7V protocol. Despite having high initial reactivity that causes Li-depletion, FEC was the only solvent to avoid increased degradation when moving to the higher termination voltage.

25 ENERGY STORAGE↗

NASA NTRS2010

Optimized Li-Ion Electrolytes Containing Fluorinated Ester Co-Solvents

A number of experimental lithium-ion cells, consisting of MCMB (meso-carbon microbeads) carbon anodes and LiNi(0.8)Co(0.2)O2 cathodes, have been fabricated with increased safety and expanded capability. These cells serve to verify and demonstrate the reversibility, low-temperature performance, and electrochemical aspects of each electrode as determined from a number of electrochemical characterization techniques. A number of Li-ion electrolytes possessing fluorinated ester co-solvents, namely trifluoroethyl butyrate (TFEB) and trifluoroethyl propionate (TFEP), were demonstrated to deliver good performance over a wide temperature range in experimental lithium-ion cells. The general approach taken in the development of these electrolyte formulations is to optimize the type and composition of the co-solvents in ternary and quaternary solutions, focusing upon adequate stability [i.e., EC (ethylene carbonate) content needed for anode passivation, and EMC (ethyl methyl carbonate) content needed for lowering the viscosity and widening the temperature range, while still providing good stability], enhancing the inherent safety characteristics (incorporation of fluorinated esters), and widening the temperature range of operation (the use of both fluorinated and non-fluorinated esters). Further - more, the use of electrolyte additives, such as VC (vinylene carbonate) [solid electrolyte interface (SEI) promoter] and DMAc (thermal stabilizing additive), provide enhanced high-temperature life characteristics. Multi-component electrolyte formulations enhance performance over a temperature range of -60 to +60 C. With the need for more safety with the use of these batteries, flammability was a consideration. One of the solvents investigated, TFEB, had the best performance with improved low-temperature capability and high-temperature resilience. This work optimized the use of TFEB as a co-solvent by developing the multi-component electrolytes, which also contain non-halogenated esters, film forming additives, thermal stabilizing additives, and flame retardant additives. Further optimization of these electrolyte formulations is anticipated to yield improved performance. It is also anticipated that much improved performance will be demonstrated once these electrolyte solutions are incorporated into hermetically sealed, large capacity prototype cells, especially if effort is devoted to ensure that all electrolyte components are highly pure.

Prakash, G. K. Surya↗

DOE OSTI2024

Deconvoluting Effects of Lithium Morphology and SEI Stability at Moderate Current Density Using Interface Engineering

Lithium (Li)-morphology and solid electrolyte interphase (SEI) are among the most significant performance regulators in Li-metal batteries (LMBs). While both Li-morphology and SEI composition play key roles in the cyclability of LMBs, less is understood about the individual contributions of each factor to overall Li reversibility, particularly at a practical current density (1 mA cm −2 ) at which the kinetics of both factors are not naturally separated. Herein, an interface engineering approach is introduced to deconvolute the impacts of Li-morphology and SEI composition on battery performance. By using interfacial nanofilms with differing resistivity (resistive HfO 2 versus conductive ZnO), the morphology of Li is varied, and by virtue of similar acidic character of the nanofilms, the formation of anion-rich SEIs is maintained. It is established that although the surface acidity of the thin films enables preformation of a more anion-rich SEI, it is not preserved after Li plating. It is further shown that resistance-controlled, low-surface-area Li-morphology exhibits up to threefold increase in stable cycle life when tested in multiple electrolytes. Overall, these findings explain why Li-morphological control is more advantageous for performance improvement than preformed SEI modulation due to the inherent challenges in SEI preservation.

36 MATERIALS SCIENCE↗

DOE OSTI2025

LiCl–Based Aqueous Electrolytes for Efficient Iron Electrodeposition

This study investigates room temperature, aqueous electrolytes for efficient iron electrodeposition. Specifically, a novel lithium chloride-based electrolyte was identified to suppress hydrogen evolution while promoting fast kinetics of iron electrodeposition, achieving high coulombic efficiency (>90%) at high current densities (>400 mA cm −2 ). Electrochemical analysis of the partial current densities of iron deposition and hydrogen co-evolution revealed that water reduction is kinetically suppressed in this electrolyte, resulting in an increase in the measured coulombic efficiency. Furthermore, a detailed investigation of the iron speciation and their complexation was performed, which revealed that, in concentrated LiCl-containing electrolytes, the ferrous (Fe 2+ ) species coordinate with chloride rather than water, enhancing deposition kinetics. The combined effect of enhanced electrodeposition kinetics and suppressed water activity provide elevated coulombic efficiency. Overall, this paper develops an understanding of anion and cation effects on the mechanism of electrodeposition and hydrogen co-evolution in concentrated electrolytes in search of improved aqueous media (e.g., concentrated LiCl) for efficient metal electro-synthesis.

Lvovich, William [Case Western Reserve University,↗

DOE OSTI2025

Electrocatalytic Reductive Amination of Aldehydes and Ketones with Aqueous Nitrite

The electrocatalytic utilization of oxidized nitrogen waste for C–N coupling chemistry is an exciting research area with great potential to be adopted as a sustainable method for generation of organonitrogen molecules. The most widely used C–N coupling reaction is reductive amination. In this work, we develop an alternative electrochemical reductive amination reaction that can proceed in neutral aqueous electrolyte with nitrite as the nitrogenous reactant and via an oxime intermediate. We develop a selection criterion for nitrite reduction electrocatalysts suited for oxime electrosynthesis and, in doing so, find Pd to be a highly efficient catalyst for this reaction, reaching an oxime Faradaic efficiency of 82% at −0.21 V vs the reversible hydrogen electrode. The aliphatic or aromatic structure of the carbonyl reactant impacts the efficacy of the catalyst, with aromatic substrates leading to suppressed oxime formation and detrimental reduction of the carbonyl to the alcohol. We developed a Pb/PbO electrocatalyst that selectively performs oxime reduction in the neutral aqueous electrolyte. With acetone as a model substrate, we demonstrate an efficient one-pot, two-step electrochemical reaction for the conversion of acetone to isopropyl amine with 85% yield and 50% global Faradaic efficiency.

catalysts↗

DOE OSTI2025

Molecular engineering of ethereal electrolyte for ultrastable Si-based high voltage full cells

The successful application of Si-based high-energy Li-ion batteries (LIBs) depends on our ability to tailor electrolyte properties to achieve long-term stability and reliable performance. In this work, we demonstrate our rationale for the molecular design of ethereal solvents to address low anodic stability issues and produce a highly electrochemically stable electrolyte for Si‖LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) high-energy full cells. Unlike the trimethylsilyl group, the trifluoromethyl (–CF 3 ) group exerts a very strong electron-withdrawing effect on the glycol ether backbone, reducing the highest occupied molecular orbital (HOMO) energy level of the fluorinated glycol ether (FGE) and significantly enhancing its oxidation potential. The FGE-based electrolyte enables stable cycling of Si‖NMC811 full cells, delivering high specific capacity (900 mA h g −1 ) and coulombic efficiency (>99.78%) over extended (500) cycles. The improved electrochemical performance originates from the terminal fluorination of the diglyme backbone, which strengthens anion coordination in the solvation structure, leading to the preferential reduction of the FSI anion and the formation of robust solid electrolyte interphases (SEIs) on the Si surface. Through molecular engineering of ethereal solvents, we have discovered a promising candidate for a next-generation stable electrolyte, paving the way for the design of practical and commercially viable Si batteries.

Silicon anode↗

DOE OSTI2026

A Quinoidal Two‐Dimensional Metal–Organic Framework for High‐Performance Micro‐Supercapacitors and Solid‐State Lithium Batteries

Two-dimensional (2D) metal-organic frameworks (MOFs) integrating redox-active linkers enable dense charge sites and open ion pathways for microscale energy storage. We report a quinoidal dicarboxylate ligand, AQM-H2L, derived from p-azaquinodimethane, forming crystalline frameworks with Cu2+ and Zn2+ nodes. The Cu-based MOF (AQM-AQM-H2L-Cu) exhibits layered sheets (>14 Å spacing) constructed from dinuclear Cu-carboxylate units and conjugated AQM linkers, which narrow the bandgap and introduce Cu2+/Cu+ pseudocapacitance. Exfoliated nanosheets (∼5 nm) retain crystallinity and excellent processability. Integrated into graphene films, they deliver areal and volumetric capacitances of 29.6 mF cm-2 and 18.1 F cm-3, achieving 2.6 mWh cm-3 energy density at 160 mW cm-3. As ionic fillers (1 wt%) in PEO solid polymer electrolytes, the nanosheets markedly enhance LiFePO4 cell performance, affording 169.8 mAh g-1 at 0.2 C and 93% retention after 400 cycles. This work establishes quinoidal linkers as a compact and robust design motif for ionically active 2D frameworks toward high-performance miniature and solid-state energy devices.

Chen, Ziman↗

DOE OSTI2024

Phloroglucinol–2,6‐Diaminoanthraquinone as a Durable Redox Mediator for Enhancing Conversion Reaction Kinetics in Lithium‐Sulfur Batteries

Abstract Lithium‐sulfur batteries, despite being a promising solution for next‐generation secondary batteries, require substantial efforts to overcome the challenges of sluggish sulfur redox kinetics, polysulfides shuttling, and Li metal instability before achieving practical viability. Conventional strategies that utilize metal catalysts or soluble redox mediators (RMs) are limited by either impractical producing processes or unsatisfactory service life. Herein, an electrochemically active organic material, phloroglucinol – 2,6‐diaminoanthraquinone (PG‐DAAQ) is synthesized through a green and facile polymerization process to better resolve these issues. Serving as an RM at the cathode, PG‐DAAQ exhibits enduring redox activity within the sulfur operating potential window, leading to enhanced redox kinetics and sulfur utilization. Remarkably, even without any metal elements, PG‐DAAQ exhibits an excellent affinity to polysulfides, thereby suppressing the shuttling and facilitating the formation of a more favorable solid‐electrolyte interface to stabilize Li deposition at the anode. As a result, Li‐S cells employing PG‐DAAQ show significantly enhanced cycling and rate performances than the control cells. Even with a low electrolyte‐to‐sulfur ratio of 6, pouch cells with PG‐DAAQ deliver a reversible discharge capacity of 821 mA h g −1 after 100 cycles at a C/10 rate.

Lai, Tianxing↗

NASA NTRS2012

Improved Wide Operating Temperature Range of LiNiCoAiO2-based Li-ion Cells with Methyl Propionate-based Electrolytes

Demonstration of wide operating temperature range Li-ion electrolytes Methyl propionate-based wide operating temperature range electrolytes were demonstrated to provide dramatic improvement of the low temperature capability of Quallion prototype Li-ion cells (MCMB-LiNiCoAlO2). Some formulations were observed to deliver over 60% of the room temperature capacity using a 5C rate at - 40oC !! Represents over a 4-fold improvement over the baseline electrolyte system. Demonstrated operational capability of a number of systems over a wide temperature range (-40 to +70 C) Demonstrated reasonably good long term cycle life performance at high temperature (i.e., at +40deg and +50 C) A number of formulations containing electrolytes additives (i.e., FEC, VC, LiBOB, and lithium oxalate) have been shown to have enhanced lithium kinetics at low temperature and promising high temperature resilience. Demonstrated good performance in larger capacity (12 Ah) Quallion Li-ion cells with methyl propionate-based electrolytes. Current efforts focused upon performing life studies and the impact upon low temperature capability.

Li-ion electrolytes↗

DOE OSTI2024

Effects of catholyte aging on high-nickel NMC cathodes in sulfide all-solid-state batteries

Sulfide solid-state electrolytes (SSEs) in all-solid-state batteries (SSBs) are recognized for their high ionic conductivity and inherent safety. The LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode offers a high thermodynamic potential of approximately 3.8 V vs. Li/Li + and a theoretical specific capacity of 200 mA h g −1 . However, the practical utilization of NMC811 in sulfide SSBs faces significant interfacial challenges. The oxidation instability of sulfide solid electrolytes against NMC811 and the formation of the cathode electrolyte interphase (CEI) during cycling lead to degradation and reduced cell performance. Volumetric changes in NMC during lithiation and de-lithiation can also cause detachment from sulfide electrolytes or internal particle cracking. Despite extensive galvanostatic cycling studies to address the issues, the calendar life of sulfide SSBs remains poorly understood. Here, we systematically studied the effects of four different catholytes on the calendar aging of LiNbO 3 (LNO)-coated NMC811, including Li 6 PS 5 Cl (LPSCl), Li 3 InCl 6 –Li 6 PS 5 Cl (LIC–LPSCl), Li 3 YCl 6 –Li 6 PS 5 Cl (LYC–LPSCl), and Li 10 GeP 2 S 12 (LGPS). Our results indicate that LPSCl provides optimal capacity retention when stored at high state-of-charge (SOC) at room temperature, but the LIC–LPSCl cathode shows significant capacity degradation and chemical incompatibility. We also established an effective electrochemical calendar aging testing protocol to simulate daily usage, enabling quick inference of the calendar life of SSBs. In conclusion, this new testing approach accelerates materials selection strategies for high-nickel NMC composite cathodes in sulfide SSBs.

25 ENERGY STORAGE↗

NASA NTRS2007

The NASA "PERS" Program: Solid Polymer Electrolyte Development for Advanced Lithium-Based Batteries

In fiscal year 2000, The National Aeronautics and Space Administration (NASA) and the Air Force Research Laboratory (AFRL) established a collaborative effort to support the development of polymer-based, lithium-based cell chemistries and battery technologies to address the next generation of aerospace applications and mission needs. The ultimate objective of this development program, which was referred to as the Polymer Energy Rechargeable System (PERS), was to establish a world-class technology capability and U.S. leadership in polymer-based battery technology for aerospace applications. Programmatically, the PERS initiative exploited both interagency collaborations to address common technology and engineering issues and the active participation of academia and private industry. The initial program phases focused on R&D activities to address the critical technical issues and challenges at the cell level. Out of a total of 38 proposals received in response to a NASA Research Announcement (NRA) solicitation, 18 proposals (13 contracts and 5 grants) were selected for initial award to address these technical challenges. Brief summaries of technical approaches, results and accomplishments of the PERS Program development efforts are presented. With Agency support provided through FY 2004, the PERS Program efforts were concluded in 2005, as internal reorganizations and funding cuts resulted in shifting programmatic priorities within NASA. Technically, the PERS Program participants explored, to various degrees over the lifetime of the formal program, a variety of conceptual approaches for developing and demonstrating performance of a viable advanced solid polymer electrolyte possessing the desired attributes, as well as several participants addressing all components of an integrated cell configuration. Programmatically, the NASA PERS Program was very successful, even though the very challenging technical goals for achieving a viable solid polymer electrolyte material or the overall envisioned long-term, program objectives were not met due to funding reductions. The NASA PERS Program provided research opportunities and generated and disseminated a wealth of new scientific knowledge and technical competencies within the polymer electrolyte area.

Baldwin, Richard S.↗

NASA NTRS2014

Lithium-Ion Electrolytes Containing Flame Retardant Additives for Increased Safety Characteristics

The invention discloses various embodiments of Li-ion electrolytes containing flame retardant additives that have delivered good performance over a wide temperature range, good cycle life characteristics, and improved safety characteristics, namely, reduced flammability. In one embodiment of the invention there is provided an electrolyte for use in a lithium-ion electrochemical cell, the electrolyte comprising a mixture of an ethylene carbonate (EC), an ethyl methyl carbonate (EMC), a fluorinated co-solvent, a flame retardant additive, and a lithium salt. In another embodiment of the invention there is provided an electrolyte for use in a lithium-ion electrochemical cell, the electrolyte comprising a mixture of an ethylene carbonate (EC), an ethyl methyl carbonate (EMC), a flame retardant additive, a solid electrolyte interface (SEI) film forming agent, and a lithium salt.

Smart, Marshall C.↗

NASA NTRS1987

Na/beta-alumina/NaAlCl4, Cl2/C circulating cell

A study was made of a high specific energy battery based on a sodium negative electrode and a chlorine positive electrode with molten AlCl3-NaCl electrolyte and a solid beta alumina separator. The basic performance of a Na beta-alumina NaAlCl4, Cl2/C circulating cell at 200 C was demonstrated. This cell can be started at 150 C. The use of melting sodium chloroaluminate electrolyte overcomes some of the material problems associated with the high working temperatures of present molten salt systems, such as Na/S and LiAl/FeS, and retains the advantages of high energy density and relatively efficient electrode processes. Preliminary investigations were conducted on a sodium-chlorine static cell, material compability, electrode design, wetting, and theoretical calculations to assure a better chance of success before assembling a Na/Cl2 circulating cell. Mathematical models provide a theoretical explanation for the performance of the NaCl2 battery. The results of mathematical models match the experimental results very well. According to the result of the mathematical modeling, an output at 180 mA/sq cm and 3.2 V can be obtained with optimized cell design.

Cherng, Jing-Yih↗

DOE OSTI2026

Modeling Single-Crystal Battery Materials: From Fundamental Understanding to Performance Evaluation

The performance of rechargeable batteries is fundamentally influenced by the physicochemical properties and microstructural features of their key material components. Recent experimental advancements have highlighted the potential of single-crystal (SC) morphologies to address inherent limitations of polycrystalline (PC) electrodes and solid-state electrolytes, offering tunable charge transport kinetics and improved cell cycling performance. Here, this review examines how state-of-the-art computational modeling, from atomistic and mesoscale to continuum-level approaches, including machine learning methodologies, has been utilized to investigate the critical factors governing the electrochemical behavior of SC battery materials. We explore how predictive modeling can elucidate the processing–structure–property–performance relationships of SC cathodes, anodes, and solid-state electrolytes, with a focus on unique SC characteristics such as crystallographic anisotropy, size effects, and facet-dependent properties. Additionally, we identify limitations in commonly used modeling techniques and discuss strategies to address these challenges. By integrating high-fidelity simulations with experimental insights, this review aims to outline a clear path for the rational design and optimization of SC battery components, paving the way for accelerated advancements in energy storage technologies.

Materials science↗