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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Surprising Relationship between Silicon Anode Calendar Aging and Electrolyte Components in a Localized High-Concentration Electrolyte System

Although localized high-concentration electrolytes (LHCEs) have been shown to improve the calendar lifetime of silicon anodes, the roles of the electrolyte constituents in calendar aging are not well understood. Here, in this work, we utilize a voltage hold protocol and an LHCE with varying molar ratios of lithium bis(fluorosulfonyl)imide (LiFSI), tetramethylene sulfone (TMS), and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) to probe the component roles during aging. Interestingly, the estimated calendar lifetime and irreversible lithium losses from the V-hold experiments are independent of the electrolyte formulations. Contrarily, the solid electrolyte interphase (SEI) composition depends on the electrolyte formulation. X-ray photoelectron spectroscopy shows that TMS-coordinated species decompose to form insoluble alkanes and lithium hydroxide (LiOH), while lithium fluoride (LiF) originates from the anion-coordination complex. The SEI composition does not appear to play a significant role in the silicon anode passivity, as measured by parasitic current, suggesting that the SEI-electrolyte interactions dictate the calendar aging mechanisms.

Si anode↗
DOE OSTI2025

Unveiling the Mechanism of Mn Dissolution Through a Dynamic Cathode‐Electrolyte Interphase on LiMn2O4

Abstract Understanding the formation and evolution of the cathode‐electrolyte interphase (CEI), which forms at the interface between the cathode and electrolyte, is crucial for revealing degradation mechanisms in cathode materials, especially for developing strategies to stabilize the interphase in the strongly oxidizing conditions that evolve at high operating voltages in next‐generation Li‐ion batteries. However, The present understanding of the CEI is challenged by its complex and dynamic nature. In this work, near‐edge X‐ray absorption fine structure spectroscopy, electrochemical characterization, and reactive molecular dynamics simulations are combined to reveal a mechanism for CEI formation and evolution above model LiMn 2 O 4 (LMO) thin‐film electrodes in contact with conventional carbonate‐based electrolytes. It is found that Mn dissolution from LMO can be understood in terms of repetitive Mn 3 O 4 formation and dissolution behavior during cycling, which is closely connected to electrolyte decomposition and a key aspect of the CEI formation and growth. The behavior of the CEI in this model system offers detailed insight into the dynamic chemistry of the interphase, underscoring the important role of electrolyte composition and cathode surface structure in interphase degradation.

Ou, Wenhan↗
DOE OSTI2025

Catalytic Electrolyte Additive for High-Loading and Lean Electrolyte Li–S Batteries

The cycle life of high-energy Li–S cells is largely constrained by the quick electrolyte depletion. LiNO 3 has been a well-established additive known for protecting the Li metal anode and stabilizing the battery from polysulfide “shuttling”. However, it can be depleted prematurely and can pose safety risks when exposed to carbon, sulfur, or Li metal under harsh conditions. Here, in this study, LiPO 2 F 2 was explored as a safe and durable alternative additive in ether-based electrolytes. LiPO 2 F 2 demonstrates superior performance in Li/S batteries, especially under high sulfur loading (∼4 mg/cm 2 ) and lean electrolyte conditions (E/S = 4), achieving a long-term cycling stability of 40%, compared to 14.7% with LiNO 3 . This additive facilitates the disproportionation of polysulfides, reducing their dissolution and mitigating the shuttle effect. Additionally, LiPO 2 F 2 promotes the formation of a stable solid-electrolyte interphase (SEI) composed of inorganic anion-derived species, improving the battery’s overall stability and functionality. These findings blaze a trail in the design of safer and more durable electrolytes for Li–S batteries.

Li-S batteries↗
DOE OSTI2025

Enhanced Reversibility of Iron Metal Anode with a Solid Electrolyte Interphase in Concentrated Chloride Electrolytes

Iron is a promising candidate for a cost-effective anode for large-scale energy storage systems due to its natural abundance and well-established mass production. Recently, Fe-ion batteries (FeIBs) that use ferrous ions as the charge carrier have emerged as a potential storage solution. The electrolytes in FeIBs are necessarily acidic to render the ferrous ions more anodically stable, allowing a wide operation voltage window. However, the iron anode suffers severe hydrogen evolution reaction with a low Coulombic efficiency (CE) in an acidic environment, shortening the battery cycle life. Herein, a hybrid aqueous electrolyte that forms a solid-electrolyte interphase (SEI) layer on the Fe anode surface is introduced. The electrolyte mainly comprises FeCl 2 and ZnCl 2 as cosalts, where the Zn-Cl anionic complex species of the concentrated ZnCl 2 allows dimethyl carbonate (DMC) to be miscible with the aqueous ferrous electrolyte. SEI derived from DMC's decomposition passivates the iron surface, which leads to an average CE of 98.3% and much-improved cycling stability. As a result, this advancement shows the promise of efficient and durable FeIBs.

25 ENERGY STORAGE↗
DOE OSTI2025

Dimolybdenum Paddlewheel Complexes with Cation Binding Sites as Electrolyte Additives to Manipulate the Solid-Electrolyte Interphase at Lithium Metal Anodes

The use of electrolyte additives at millimolar loadings to control the surface chemistry of lithium metal anodes (LMAs) is a leading strategy to improve lithium metal batteries and promote electrosynthetic reactions. Whereas previous studies employed either inorganic or organic additives, in this study, we report the first organometallic additive, Mo 2 (mea) 4 [1, mea = 2-(2-methoxyethoxy)acetate], a dimolybdenum paddlewheel complex that is stable under Li plating conditions and features cation binding sites in the second coordination sphere that promote reversible Li + coordination. Binding of Li + ions to 1 induces immobilization of cationically charged aggregates (or products thereof) into the solid electrolyte interphase (SEI), imparting multiple beneficial functions. The modified SEI was found to protect the LMA against parasitic side reactions, produce modest but measurable improvements to Li plating properties (e.g., overpotential, surface structure, and Coulombic efficiency), and improve interfacial charge transport properties. Furthermore, the most notable benefit to battery cycling performance appears in calendar aging tests, which show that the presence of the additive protects the LMA from parasitic side reactions that would otherwise decrease overall cell cycling efficiency over time. Collectively, these data disclose a tactic for designing electrolyte additives using principles of organometallic synthesis.

Additives↗
DOE OSTI2026

Investigation Into LiCl-LiF+Li 2 O as a Low Temperature Electrolyte in Direct Electrolytic Reduction of UO 2

Direct electrolytic reduction (DER) of UO 2 in a binary LiCl-Li2O (1–3 wt%) at 650 °C has been widely reported. The process temperature can be reduced to 550 °C in theory by using a near eutectic ternary LiCl-LiF+Li 2O (∼2 wt%) electrolyte, which will result in substantial reduction in rate of salt vaporization. The feasibility of using the ternary electrolyte for the process was tested via material compatibility testing, electrochemical polarization testing, and controlled potential or current DER experiments. MgO, Pt, and 625 nickel samples were each contacted with the ternary salt for 168 h. Negligible changes to dimensions and mass of the samples were measured, and concentrations of corrosion products in the salt were 102 ppm or less. O2−oxidation was observed to occur at a lower potential than Cl-or F-on a Pt anode. DER of UO2was performed in six trials. Process variables included type of reference electrode, electrochemical control method, type of cathode basket, and electrolyte composition. UO 2conversion ranged from 28.2 to 99.9 % , and current efficiency ranged from 38 to 52%. Overall, results indicate that the use of the ternary salt is feasible for DER.

36 MATERIALS SCIENCE↗
NASA NTRS2003

Preliminary Evaluations of Polymer-based Lithium Battery Electrolytes Under Development for the Polymer Electrolyte Rechargeable Systems Program

A component screening facility has been established at The NASA Glenn Research Center (GRC) to evaluate candidate materials for next generation, lithium-based, polymer electrolyte batteries for aerospace applications. Procedures have been implemented to provide standardized measurements of critical electrolyte properties. These include ionic conductivity, electronic resistivity, electrochemical stability window, cation transference number, salt diffusion coefficient and lithium plating efficiency. Preliminary results for poly(ethy1ene oxide)-based polymer electrolyte and commercial liquid electrolyte are presented.

Manzo, Michelle A.↗
DOE OSTI2026

Precious metal oxygen-evolving anodes for electrolytic reduction of metal oxides in molten LiCl-Li 2 O electrolyte

Understanding the electrochemical stability of oxygen-evolving anode materials in molten salt electrolytes is essential to enable decarbonized electrolytic reduction of metal oxides (e.g., used nuclear oxide fuels). Here, this work investigated three precious metals (Ir, Ru, and Pt) as oxygen-evolving anodes in molten LiCl-Li 2 O (99.0-1.0 wt%) at 650 °C. For consistent measurements, this work employed a three-electrode cell comprised of a two-phase Li-Bi (65-35 at%) reference electrode and a NiO counter electrode. Anodic polarization behavior of each anode was investigated via cyclic voltammetry (CV) and chronoamperometry. The onset potential for oxygen evolution was observed at E > 2.9 V (vs. Li/Li + ) for the Ir and Ru anodes and anodic current density was as high as 1.0 A cm -2 at 3.23 V. The dimensional stability of each anode was evaluated from long-term electrolysis experiments (10.0-32.1 h) at 3.23 V. Rapid consumption of the Pt anode was observed after the application of 26,453 C cm -2 with a reduction in diameter of about 15.8% due to the formation of a non-protective Li 2 PtO 3 compound. The formation of this compound was also observed during CV measurements as additional anodic waves at potentials more negative than that of oxygen evolution. In contrast, both the Ir and Ru anodes exhibited excellent dimensional stability with a reduction in diameter or thickness of less than 1.5% even after applying greater charge density of ~41,100 C cm -2 , demonstrating superior stability during oxygen evolution in the LiCl-Li 2 O electrolyte.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Investigation of electrode-electrolyte interfaces to enable non-flammable Li-ion batteries operating up to 125°C with liquid electrolyte

Non-flammable and high-temperature stable ionic liquid (IL)-based electrolytes could eliminate catastrophic battery failures and improve battery safety, but their poor electrochemical interaction with the LiNi x Mn y Co z O 2 (NMC) family of cathodes is a long-standing problem due to severe parasitic reactions at high temperature. Understanding surface and bulk structural mechanisms of NMC-type cathodes at elevated operational temperature is of paramount importance to facilitate stable electrochemical performance. Here, we report a non-flammable phosphonium IL-based cell chemistry that offers stable electrode-electrolyte interfaces, leading to electrochemical performance up to 125°C and high-temperature safety. We combine electrochemistry with multimodal X-ray spectroscopy methods to understand interfaces at elevated temperature (100°C). This nanoscale understating enables a proof-of-concept high-temperature cylindrical cell (14500), and the design achieves an average Coulombic efficiency of ≈99.5% up to 300 cycles at 100°C. The results ascertain the significance of depth-dependent degradation at the interface, guiding room-temperature Li-ion technology toward extreme-temperature applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Control of Two Solid Electrolyte Interphases at the Negative Electrode of an Anode‐Free All Solid‐State Battery based on Argyrodite Electrolyte

Abstract Anode‐free all solid‐state batteries (AF‐ASSBs) employ “empty” current collector with three active interfaces that determine electrochemical stability; lithium metal – Solid electrolyte (SE) interphase (SEI‐1), lithium – current collector interface, and collector – SE interphase (SEI‐2). Argyrodite Li 6 PS 5 Cl (LPSCl) solid electrolyte (SE) displays SEI‐2 containing copper sulfides, formed even at open circuit. Bilayer of 140 nm magnesium/30 nm tungsten (Mg/W‐Cu) controls the three interfaces and allows for state‐of‐the‐art electrochemical performance in half‐cells and fullcells. AF‐ASSB with NMC811 cathode achieves 150 cycles with Coulombic efficiency (CE) above 99.8%. With high mass‐loading cathode (8.6 mAh cm −2 ), AF‐ASSB retains 86.5% capacity after 45 cycles at 0.2C. During electrodeposition of Li, gradient Li‐Mg solid solution is formed, which reverses upon electrodissolution. This promotes conformal wetting/dewetting by Li and stabilizes SEI‐1 by lowering thermodynamic driving force for SE reduction. Inert refractory W underlayer is required to prevent ongoing formation of SEI‐2 that also drives electrochemical degradation. Inert Mo and Nb layers likewise protect Cu from corroding, while Li‐alloying layers (Mg, Sn) are less effective due to ongoing volume changes and associated pulverization. Mechanistic explanation for observed Li segregation within alloying Li x Mg layer is provided through mesoscale modelling, considering opposing roles of diffusivity differences and interfacial stresses.

Wang, Yixian [Materials Science and Engineering Pr↗
NASA NTRS1993

The electrolyte challenge for a direct methanol-air polymer electrolyte fuel cell operating at temperatures up to 200 C

Novel polymer electrolytes are being evaluated for use in a direct methanol-air fuel cell operating at temperatures in excess of 100 C. The evaluation includes tests of thermal stability, ionic conductivity, and vapor transport characteristics. The preliminary results obtained to date indicate that a high temperature polymer electrolyte fuel cell is feasible. For example, Nafion 117 when equilibrated with phosphoric acid has a conductivity of at least 0.4 Omega(exp -1)cm(exp -1) at temperatures up to 200 C in the presence of 400 torr of water vapor and methanol vapor cross over equivalent to 1 mA/cm(exp 2) under a one atmosphere methanol pressure differential at 135 C. Novel polymers are also showing similar encouraging results. The flexibility to modify and optimize the properties by custom synthesis of these novel polymers presents an exciting opportunity to develop an efficient and compact methanol fuel cell.

Savinell, Robert↗
NASA NTRS1973

Electrolytic hydrogen fuel production with solid polymer electrolyte technology.

A water electrolysis technology based on a solid polymer electrolyte (SPE) concept is presented for applicability to large-scale hydrogen production in a future energy system. High cell current density operation is selected for the application, and supporting cell test performance data are presented. Demonstrated cell life data are included to support the adaptability of the SPE system to large-size hydrogen generation utility plants as needed for bulk energy storage or transmission. The inherent system advantages of the acid SPE electrolysis technology are explained. System performance predictions are made through the year 2000, along with plant capital and operating cost projections.

Titterington, W. A.↗
NASA NTRS1985

Description, validation, and modification of the Guyton model for space-flight applications. Part A. Guyton model of circulatory, fluid and electrolyte control. Part B. Modification of the Guyton model for circulatory, fluid and electrolyte control

The mathematical model that has been a cornerstone for the systems analysis of space-flight physiological studies is the Guyton model describing circulatory, fluid and electrolyte regulation. The model and the modifications that are made to permit simulation and analysis of the stress of weightlessness are described.

Leonard, J. I.↗
DOE OSTI2026

Role of electrolyte in silicon electrolyte interface stabilization

Transition metal ion dissolution was long thought to be the reason for poor cycling performance in Lithium ion batteries cycled to a high voltage, but since the anode SEI is electrochemically insulating, the mechanism for transition metal mediated SEI decomposition in unclear. Our results show that acidic species such as F 2 PO 2 H generation on the cathode side and their subsequent crossover reactions with the SEI components damaging it could more likely be a major factor to capacity fade.

25 ENERGY STORAGE↗
DOE OSTI2025

Thermal decomposition pathways of bulk electrolytes on vanadium oxide nanocrystals

The thermal stability of electrolytes at an elevated temperature induced by battery charge-discharge cycling is critical for the long cycling performance of a rechargeable battery. For many multivalent systems, such as rechargeable magnesium batteries, which offer great potential for high energy density and utilize earth-abundant resources, electrolyte instability and electrode surface passivation, arising from electrolyte decomposition, remain as major roadblocks. Understanding the electrolyte decomposition pathways at the electrode-electrolyte interface is essential to provide guidance in overcoming this challenge. In this work, in situ 13 C magic angle spinning nuclear magnetic resonance (MAS NMR) and first-principles calculations were used to investigate the thermal decomposition of the electrolyte in a system consisting of MgV 2 O 4 , a novel cathode for magnesium batteries, mixed with a bulk electrolyte consisting of magnesium bis(trifluoromethanesulfonyl)imide (Mg(TFSI) 2 ) in diglyme (G2). We show that significant electrolyte decomposition is observed in bulk 1.0 M Mg(TFSI) 2 in G2 mixed with nanometer sized MgV 2 O 4 powder at elevated temperatures. This observation is to mimic the possible thermal decomposition that might happen during battery cycling. We demonstrate that the MgV 2 O 4 surface is covered by a layer of decomposed G2 products. We conclude that the dominant reaction pathway for electrolyte decomposition is the thermal decomposition of the pure electrolytes at elevated temperatures, followed by adsorption of G2 decomposition products to the MgV 2 O 4 surface. The activation energy for the major decomposition pathway is obtained. In conclusion, this work highlights the importance of studying thermal decomposition of electrolytes for overall system stability and explores electrolyte stability at significantly elevated temperatures.

25 ENERGY STORAGE↗