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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Interlayer Design for Halide Electrolytes in All‐Solid‐State Lithium Metal Batteries

Abstract All‐solid‐state lithium‐metal batteries (ASSLMBs) are promising for transportation electrification due to their superior safety and high energy density. Lithium halide electrolytes provide excellent processing flexibility, high ionic conductivity, and anodic stability (>4.1 V), making them highly compatible with high‐voltage cathodes, surpassing sulfide electrolytes (<2.1 V). Nevertheless, halide electrolytes suffer from low cathodic stability and form an electronically conductive interphase with lithium, resulting in a critical current density (CCD) of nearly zero. Herein, Li 3 YbCl 6 electrolytes are synthesized that are kinetically stable with lithium by forming an electronic insulating solid electrolyte interphase. Guided by critical overpotential criteria, a PI 3 interlayer is designed that transforms into Li 6 PI 3 upon contact with lithium, substantially reducing the interfacial resistance of Li 3 YbCl 6 against lithium to 34 Ω and achieving a high critical overpotential of 114 mV. By substituting Yb with Lu, Li 3 LuCl 6 electrolytes with Li 6 PI 3 interlayers reach a CCD of 1.0 mA cm −2 at a capacity of 1.0 mAh cm −2 , comparable to sulfide electrolytes but with higher oxidation stability. Additionally, Li 6 PI 3 enables stable cycling of Li//Li cells with Li 3 LuCl 6 electrolytes at 0.5 mA cm −2 for 400 cycles and maintains 86.5% capacity in Li//LiCoO 2 cells after 220 cycles at 30 °C, paving the way for high‐performance ASSLMBs.

Chemistry↗
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 OSTI2023

Na 3 Zr 2 Si 2 PO 12 Solid Electrolyte Membrane for High‐Performance Seawater Battery

Abstract Seawater batteries (SWBs) have gained tremendous interest in the electrochemical energy storage research field because of their low cost, natural abundance, and potential use for long‐duration energy storage. Advancing a SWB to demonstration projects is plagued by the poor electrochemical performance stemming from the poor interfaces of the solid electrolyte (SE), as well as the structural and chemical instabilities and sluggish ionic transport properties. In this study, the anode compartment of a surrogate SWB is constructed with a Na | SE | hard carbon configuration, and tailored dopants are introduced into the Nasicon‐type Na 3 Zr 2 Si 2 PO 12 (NZSP) SE membrane. After doping with TiO 2 , a much more densely packed pellet with uniformly distributed porous structure is obtained. Changes in surface chemistry and local structure in the bulk are observed, which are believed to contribute to the improved ionic conductivity and higher critical current density of the TiO 2 ‐doped NZSP. Stable cycling performance with reversible capacities based on different Na storage mechanisms are also demonstrated.

25 ENERGY STORAGE↗
DOE OSTI2025

Green Electrode Processing Enabled by Fluoro-Free Multifunctional Binders for Lithium-Ion Batteries

The eco-friendly processing of conjugated polymer binder for lithium-ion batteries demands improved polymer solubility by introducing functional moieties, while this strategy will concurrently sacrifice polymer conductivity. Employing the polyfluorene-based binder poly(2,7-9,9 (di(oxy-2,5,8-trioxadecane))fluorene) (PFO), soluble in water-ethanol mixtures, a novel approach is presented to solve this trade-off, which features integration of aqueous solution processing with subsequent controlled thermal-induced cleavage of solubilizing side chains, to produce hierarchically ordered structures (HOS). The thermal processing can enhance the intermolecular π–π stacking of polyfluorene backbone for better electrochemical performance. Notably, HOS-PFO demonstrated a substantial 6–7 orders of magnitude enhancement in electronic conductivity, showcasing its potential as a functional binder for lithium-ion batteries. As an illustration, HOS-PFO protected SiOx anodes, utilizing in situ side chain decomposition of PFO surrounding SiOx particles after aqueous processing are fabricated. HOS-PFO contributed to the stable cycling and high-capacity retention of practical SiOx anodes (3.0 mAh cm -2 ), without the use of any conducting carbon additives or fluorinated electrolyte additives. It is proposed that this technique represents a universal approach for fabricating electrodes with conjugated polymer binders from aqueous solutions without compromising conductivity.

25 ENERGY STORAGE↗
DOE OSTI2020

A Metal Organic Framework Derived Solid Electrolyte for Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSBs) are currently considered as promising candidates for next-generation energy storage technologies. However, their practical application is hindered by the critical issue of the polysulfide-shuttle. Herein, a metal organic framework (MOF)-derived solid electrolyte is presented to address it. The MOF solid electrolyte is developed based on a Universitetet i Oslo (UIO) structure. By grafting a lithium sulfonate (-SO 3 Li) group to the UIO ligand, both the ionic conductivity and the polysulfide-suppression capability of the resulting -SO 3 Li grafted UIO (UIOSLi) solid electrolyte are greatly improved. After integrating a Li-based ionic liquid (Li-IL), lithium bis(trifluoromethanesulfonyl)imide in 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, the resulting Li-IL/UIOSLi solid electrolyte exhibits an ionic conductivity of 3.3 × 10 -4 S cm -1 at room temperature. Based on its unique structure, the Li-IL/UIOSLi solid electrolyte effectively restrains the polysulfide shuttle and suppresses lithium dendritic growth. Lithium–sulfur cells with the Li-IL/UIOSLi solid electrolyte and a Li 2 S 6 catholyte show stable cycling performance that preserves 84% of the initial capacity after 250 cycles with a capacity-fade rate of 0.06% per cycle.

25 ENERGY STORAGE↗
DOE OSTI2023

Decoupling Accurate Electrochemical Behaviors for High-Capacity Electrodes via Reviving Three-Electrode Vehicles

Developing high-capacity electrodes requires the evaluation of electrochemical behaviors with an increasing current density. Currently, the current density for evaluation of high-capacity electrodes has reached a new stage where the polarization at the lithium counter electrode has become a technical barrier for the accurate evaluation of battery electrodes, resulting in severe performance and mechanism mischaracterizations. Here, the accurate electrochemical behavior for high-capacity electrodes via a single-channel three-electrode vehicle is decoupled, by which the impact of lithium counter electrode is minimized. The testing high-capacity graphite electrode is capable of delivering an excellent rate capability with 81.7% capacity retention at 0.3 C, as well as stable cycling performance retaining 97.5% practical reversible capacity after 225 cycles, much higher than the graphite electrode tested with traditional half-cell testing vehicle but in close agreement with the results obtained from a well-matched full cell, reflecting accurate electrochemical performance evaluations of high-capacity electrodes. Moreover, detailed electrochemical mechanisms of impedance and diffusion properties for working electrodes are also successfully decoupled individually. Here, this work uncovers the mismatch between traditional evaluation configuration and increasing testing current density and provides a guideline for accurate electrochemical evaluation for ever-increasing high-capacity electrodes, which is of great significance for high-energy lithium or other alkali-metal ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Strategically Modified Ligand Incorporating Mixed Phosphonate and Carboxylate Groups to Enhance Performance in All-Iron Redox Flow Batteries

Iron redox flow batteries (Fe-RFBs) hold significant promise for achieving cost-effectiveness and utilizing abundant materials for stationary energy storage applications. Here, a design of a novel Fe complex utilizing a nitrogenous phosphonate/carboxylate mixed ligand, N,N-Bis(phosphonomethyl)glycine (BMPG), is presented to achieve high performance Fe anolyte. Compared to its all-phosphonate form, nitrilotri(methylphosphonic acid) (NTMPA), the new complex Fe(BPMG) 2 demonstrates a negatively shifted redox potential, resulting in ≈0.07 V (≈10%) increase in battery output voltage. Full battery testing paired with ferrocyanide catholyte demonstrates stable cycling (capacity degradation <0.0001%/cycle) over 730 consecutive charge/discharge cycles with Coulombic Efficiency of 100% at a current density of 20 mA cm -2 under near neutral pH (≈8). Of particular interest, density functional theory (DFT) studies and operando Raman measurements provide strong evidence supporting a molecular structure in BPMG, which reveals the mixed phosphonate/carboxylate groups in BPMG maintain the octahedral coordination of the Fe ion center with phosphonates exclusively, while leaving the carboxylate unbound for both Fe(II) and Fe(III) complexes. This structural similarity between BPMG-based Fe(II) and Fe(III) complexes effectively mitigates the slow redox reaction kinetics observed in Fe(NTMPA) 2 anolyte, where significant ligand reorientation occurs between Fe(II) and Fe(III) complexes.

25 ENERGY STORAGE↗
DOE OSTI2025

Alternative Solid‐State Synthesis Route for Highly Fluorinated Disordered Rock‐Salt Cathode Materials for High‐Energy Lithium‐Ion Batteries

Abstract Fluorination has been identified as a key element for enabling the stable cycling of earth‐abundant manganese‐based disordered rock salt (DRX) cathodes. However, fluorination in the DRX bulk remains a challenge for scalable solid‐state synthesis. In this study, a tailored reaction pathway is proposed to synthesize a highly fluorinated DRX. It is demonstrated for the first time that the unconventional precursors, Li 6 MnO 4 , MnF 2 , and TiO 2 , can avoid the formation of Mn‐based intermediates (such as Li 2 (Mn,Ti)O 3, LiMnO 2 , and Mn 3 O 4 ), which, once formed, persist until the synthesis temperature reaches close to or above that required for fluorine volatility. Therefore, this method can form a highly fluorinated DRX with a composition of Li 1.23 Mn 0.40 Ti 0.37 O 2−y F y ( y = 0.29–0.34) at a low temperature (800 °C) relative to that required for conventional DRX solid‐state reactions (≥900 °C). Li 1.23 Mn 0.40 Ti 0.37 O 2−y F y ( y = 0.29–0.34) delivers a specific capacity above 300 mAh g −1 and a specific energy of 980 Wh kg −1 at 30 °C. Detailed characterization reveals that this DRX phase reversibly utilizes Mn 2+/3+ redox in the low‐voltage region and Mn 3+/4+ redox in the middle‐voltage range, whereas reversible oxygen redox is observed at high potentials.

Avvaru, Venkata Sai↗
DOE OSTI2022

From Copper to Basic Copper Carbonate: A Reversible Conversion Cathode in Aqueous Anion Batteries

Abstract Dual‐ion batteries that use anions and cations as charge carriers represent a promising energy‐storage technology. However, an uncharted area is to explore transition metals as electrodes to host carbonate in conversion reactions. Here we report the reversible conversion reaction from copper to Cu 2 CO 3 (OH) 2 , where the copper electrode comprising K 2 CO 3 and KOH solid is self‐sufficient with anion‐charge carriers. This electrode dissociates and associates K + ions during battery charge and discharge. The copper active mass and the anion‐bearing cathode exhibit a reversible capacity of 664 mAh g −1 and 299 mAh g −1 , respectively, and relatively stable cycling in a saturated mixture electrolyte of K 2 CO 3 and KOH. The results open an avenue to use carbonate as a charge carrier for batteries to serve for the consumption and storage of CO 2 .

Gallagher, Trenton C.↗
DOE OSTI2022

Highly Efficient Organosulfur and Lithium‐Metal Hosts Enabled by C@Fe 3 N Sponge

Abstract Lithium‐organosulfur (Li‐OS) batteries, despite possessing high theoretical specific capacity, encounter a few practical challenges, including unsatisfactory lifespan and low active material utilization under realistic conditions. Here, diisoropyl xanthogen polysulfide (DIXPS) has been selected as a model organosulfur compound to investigate the practical feasibility of Li‐OS batteries under realistic conditions. A well‐designed freestanding carbon sponge decorated with Fe 3 N nanoparticles (C@Fe 3 N) is introduced into the Li‐OS cells as a scaffold for both Li and DIXPS. The lithiophilic property of the C@Fe 3 N host guides uniform lithium deposition at the anode, and the catalysis of the DIXPS conversion reaction promotes the kinetics at the cathode. Impressively, the synergistic effect of C@Fe 3 N leads to an extremely stable cycling performance over 1 000 cycles in a Li‐OS full cell under realistic conditions.

He, Jiarui↗
DOE OSTI2022

Ultrafast Metal Electrodeposition Revealed by In Situ Optical Imaging and Theoretical Modeling towards Fast–Charging Zn Battery Chemistry

Metallic Zn is a preferred anode material for rechargeable aqueous batteries towards a smart grid and renewable energy storage. Importantly, understanding how the metal nucleates and grows at the aqueous Zn anode is a critical and challenging step to achieve full reversibility of Zn battery chemistry, especially under fast-charging conditions. Here, by combining in situ optical imaging and theoretical modeling, we uncover the critical parameters governing the electrodeposition stability of the metallic Zn electrode, that is, the competition among crystallographic thermodynamics, kinetics, and Zn 2+ -ion diffusion. Moreover, steady-state Zn metal plating/ stripping with Coulombic efficiency above 99 % is achieved at 10-100 mA cm -2 in a reasonably high concentration (3 M) ZnSO 4 electrolyte. Significantly, a long-term cycling-stable Zn metal electrode is realized with a depth of discharge of 66.7% under 50 mA cm -2 in both Zn || Zn symmetrical cells and MnO 2 || Zn full cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

From Copper to Basic Copper Carbonate: A Reversible Conversion Cathode in Aqueous Anion Batteries

Dual-ion batteries that use anions and cations as charge carriers represent a promising energy-storage technology. However, an uncharted area is to explore transition metals as electrodes to host carbonate in conversion reactions. Here we report the reversible conversion reaction from copper to Cu 2 CO 3 (OH) 2 , where the copper electrode comprising K 2 CO 3 and KOH solid is self-sufficient with anion-charge carriers. This electrode dissociates and associates K + ions during battery charge and discharge. The copper active mass and the anion-bearing cathode exhibit a reversible capacity of 664 mAh g –1 and 299 mAh g –1 , respectively, and relatively stable cycling in a saturated mixture electrolyte of K 2 CO 3 and KOH. Finally, the results open an avenue to use carbonate as a charge carrier for batteries to serve for the consumption and storage of CO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Enhancing Li + Transport in NMC811||Graphite Lithium–Ion Batteries at Low Temperatures by Using Low–Polarity–Solvent Electrolytes

LiNi x Co y MnzO 2 (x+y+z=1)||graphite lithium-ion battery (LIB) chemistry promises practical applications. However, its low-temperature (≤ –20°C) performance is poor because the increased resistance encountered by Li + transport in and across the bulk electrolytes and the electrolyte/electrode interphases induces capacity loss and battery failures. Though tremendous efforts have been made, there is still no effective way to reduce the charge transfer resistance (R ct ) which dominates low-temperature LIBs performance. In this work, we propose a strategy of using low-polarity-solvent electrolytes which have weak interactions between the solvents and the Li + to reduce R ct , achieving facile Li + transport at sub-zero temperatures. The exemplary electrolyte enables LiNi 0.8 Mn 0.1 Co 0.1 O 2 ||graphite cells to deliver a capacity of ≈113 mAh g –1 (98% full-cell capacity) at 25°C and to remain 82% of their room-temperature capacity at –20°C without lithium plating at 1/3C. They also retain 84% of their capacity at –30°C and 78% of their capacity at –40°C and show stable cycling at 50°C.

25 ENERGY STORAGE↗
DOE OSTI2022

Highly Efficient Organosulfur and Lithium-Metal Hosts Enabled by C@Fe 3 N Sponge

Lithium-organosulfur (Li-OS) batteries, despite possessing high theoretical specific capacity, encounter a few practical challenges, including unsatisfactory lifespan and low active material utilization under realistic conditions. Here, diisoropyl xanthogen polysulfide (DIXPS) has been selected as a model organosulfur compound to investigate the practical feasibility of Li-OS batteries under realistic conditions. A well-designed freestanding carbon sponge decorated with Fe 3 N nanoparticles (C@Fe 3 N) is introduced into the Li-OS cells as a scaffold for both Li and DIXPS. The lithiophilic property of the C@Fe 3 N host guides uniform lithium deposition at the anode, and the catalysis of the DIXPS conversion reaction promotes the kinetics at the cathode. Impressively, the synergistic effect of C@Fe 3 N leads to an extremely stable cycling performance over 1000 cycles in a Li-OS full cell under realistic conditions.

25 ENERGY STORAGE↗
DOE OSTI2023

High‐Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All‐Solid‐State Batteries

Abstract Superionic solid electrolytes (SEs) are essential for bulk‐type solid‐state battery (SSB) applications. Multicomponent SEs are recently attracting attention for their favorable charge‐transport properties, however a thorough understanding of how configurational entropy (ΔS conf ) affects ionic conductivity is lacking. Here, we successfully synthesized a series of halogen‐rich lithium argyrodites with the general formula Li 5.5 PS 4.5 Cl x Br 1.5‐x (0≤x≤1.5). Using neutron powder diffraction and 31 P magic‐angle spinning nuclear magnetic resonance spectroscopy, the S 2− /Cl − /Br − occupancy on the anion sublattice was quantitatively analyzed. We show that disorder positively affects Li‐ion dynamics, leading to a room‐temperature ionic conductivity of 22.7 mS cm −1 (9.6 mS cm −1 in cold‐pressed state) for Li 5.5 PS 4.5 Cl 0.8 Br 0.7 (ΔS conf =1.98R). To the best of our knowledge, this is the first experimental evidence that configurational entropy of the anion sublattice correlates with ion mobility. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors by tailoring the degree of compositional complexity. Moreover, the Li 5.5 PS 4.5 Cl 0.8 Br 0.7 SE allowed for stable cycling of single‐crystal LiNi 0.9 Co 0.06 Mn 0.04 O 2 (s‐NCM90) composite cathodes in SSB cells, emphasizing that dual‐substituted lithium argyrodites hold great promise in enabling high‐performance electrochemical energy storage.

Chemistry↗
DOE OSTI2026

Modulating Li + and Polysulfide Solvation with Low-Density Moderately Solvating Electrolytes for Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries show great promise as the next-generation rechargeable batteries, yet they still suffer from polysulfide shuttling and interphasial instability. Electrolyte, as the medium for ion transport and sulfur conversion, plays a crucial role in overcoming these challenges. Here, we introduce a moderately solvating electrolyte (MSE) based on low-density, low-viscosity, and nonfluorinated ether co-solvents that balances polysulfide suppression, Li metal stabilization, and redox kinetics. Through multiple solvent–solvent and solvent-ion interactions, the optimized MSE weakens Li + -solvent pairing while strengthening cation–anion interactions, thereby lowering the desolvation barrier and promoting the formation of a favorable solid–electrolyte interphase (SEI). Meanwhile, MSE limits the polysulfide dissolution but improves the accessibility of active material through better wettability and tailored solvation environment, leading to an altered sulfur deposition mechanism with β – α conversion. This approach enables a stable cycling of high-mass loading Li–S cells (> 3.5 mg cm -2 ) at both room temperature and 45 °C (where shuttling and side reactions are severer), and demonstrates a pouch cell with lean electrolyte content (4.5 µL mg s -1 ). This work highlights a practical route to develop high-performance electrolyte for Li–S cells and provides mechanistic insights into their operation.

25 ENERGY STORAGE↗
DOE OSTI2026

Humins-Derived Hard Carbon as a Low-Cost Material for Sodium-Ion Battery Anodes

The growing demand for sodium-ion batteries (SIBs) in grid storage underscores the need for electrode materials that balance performance and cost, including sustainable and robust carbon sources. The equitable and abundant distribution of materials for SIBs, along with their superior low-temperature performance, safety, and fast-charging capability, further distinguishes them from lithium-ion batteries (LIBs). Hard carbon (HC) is the state-of-the-art anode for SIBs, but current commercial HC production is localized mostly to one region of the world, raising concerns about supply chain vulnerability, critical material dependency, and environmental aspects. Here, the first demonstration of humins, an abundant biorefinery byproduct, as a precursor for HC anodes for sodium-ion storage is reported. Humins were carbonized at 1100 degrees C-1300 degrees C, and the resulting materials were subjected to comprehensive materials and electrochemical characterization. Among the temperatures studied, humins-derived hard carbon synthesized at 1200 degrees C delivers an initial reversible capacity 270mA h g-1 , with stable cycling performance up to 500 cycles and excellent rate capability, representing the optimal performance. This study establishes humins as a promising and low-cost carbon source that provides a route to mitigate supply chain risks and valorizes an underutilized biorefinery waste stream for high-performance SIB anodes.

25 ENERGY STORAGE↗
DOE OSTI2025

Fluorinated Rocksalt‐Polyanion Cathode for Lithium‐Ion Batteries

Integrated rocksalt‐polyanion cathodes (DRXPS) are promising candidates for next‐generation lithium‐ion battery cathode materials that combine high energy density, stable cycling performance, and reduced reliance on Co and Ni. In this work, we investigated Li 3 Mn 1.6 P 0.4 O 5.4 F 0.6 , a new DRXPS cathode with fluoride incorporation. A pure spinel phase was formed and a discharge capacity retention of 84% was achieved after 200 cycles between 1.5 and 4.8 V versus Li/Li + . In comparison, the similarly synthesized Li 3 Mn 1.6 Nb 0.4 O 5.4 F 0.6 , in which all P 5+ was substituted by Nb 5+ while maintaining the same stoichiometry for all other elements, crystallized in a disordered rocksalt structure, and exhibited inferior capacity retention and rate capability than the P 5+ counterpart. Our findings expand the compositional space of DRXPS to include F − , justify the viability of integrating polyanion groups in rocksalt‐type cathodes, and highlight the superiority of P 5+ as a cation charge compensator compared to the commonly used Nb 5+ . This work thereby advances the design of robust, high‐performance cathode materials for sustainable batteries.

36 MATERIALS SCIENCE↗