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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Scalable Surface Micro-Texturing of LLZO Solid Electrolytes for Battery Applications

A challenge for lithium lanthanum zirconate (LLZO)-based solid-state batteries is to increase the critical current density (CCD) to enable high current cycling. A promising strategy is to modify the LLZO surface morphology to provide a larger contact area with the Li metal. Here, a surface-textured thin LLZO electrolyte was prepared through an easily scalable process. The texturing process is a simple pressing of green LLZO tapes between micro-textured substrates. A variety of textures can be produced, depending on the type of substrate, and texturing can be on either one side or both sides. For this work, after pressing and sintering, several micro-patterns are formed on thin LLZO (~118 μm thick). The properties of the various samples were characterized to investigate the impact of surface texturing, and the most promising ones were selected for electrochemical testing in symmetrical lithium cells and full cells. Li symmetric cells using a coarse ridge-textured LLZO exhibit ~2.5 times increased CCD compared to planar non-textured LLZO, and a solid-state full cell shows stable cycling and improved rate performance. Finally, we believe this process offers a favorable trade-off of processing complexity vs structural optimization to maximize CCD.

25 ENERGY STORAGE↗
DOE OSTI2023

High-throughput and high-performance lithium-ion batteries via dry processing

A scalable powder-to-electrode dry processing strategy mainly based on powder dry mixing and rolling/calendering is rationally designed. The dry processed electrodes show lower tortuosity compared to that of conventional slurry-based electrodes. The dry-processed high-loading graphite anodes (6.6 mAh cm -2 ) and LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathodes (6.0 mAh cm -2 ) exhibit promising electrochemical performance in half-cells and full-cells. The full-cells with both electrodes from dry processing demonstrates superb rate performance to their counterpart with conventional slurry-based electrodes and delivers of capacity retentions of 74.1 % and 63.6 % over 400 and 800 cycles, respectively. Notably, the initial Coulombic efficiency of the dry processed graphite anodes is low ascribed to polytetrafluoroethylene binder. Finally, the results suggest that dry processing is promising for future lithium-ion battery manufacturing and also pinpoint the needs of modification for the polytetrafluoroethylene binder in the graphite anodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

From Pyrolysis Oil to Advanced Biographite Anode: Unravelling Biocoke Structural Evolution and Delayed Coking Effects

Catalytic graphitization of biomass-derived carbon offers a promising route to produce biographite as a sustainable alternative to petroleum-based synthetic graphite for lithium-ion battery (LIB) anodes. This study investigates the physicochemical properties of biocokes produced from pyrolysis oil at carbonization temperatures ranging from 150 degrees C to 500 degrees C. Using an iron (Fe) catalyst, graphitization was performed at 1500 degrees C, significantly lower than the ~3000 degrees C required for conventional synthetic graphite. The effects of introducing an intermediate-temperature hold (400 degrees C-600 degrees C) prior to graphitization were evaluated, simulating a "delayed coking" process to enable the coproduction of sustainable aviation fuels (SAFs). Chemical structure evolution during biocoke formation was analyzed, and proposed mechanisms are presented. Biographites produced via the delayed coking pathway exhibited high crystallinity and excellent electrochemical performance in both half-cell and full-cell LIB configurations. The full cells exhibited an initial discharge capacity close to the theoretical capacity of the NMC622 cathode (175 mAh/g at 4.2 V), and high capacity retention (~88%) after 150 cycles. Notably, the graphitic and electrochemical properties remained stable across the range of intermediate hold temperatures. These findings provide a foundation for optimizing temperature parameters in delayed coking systems to enable scalable, integrated production of biographite and SAFs from pyrolysis oil.

09 BIOMASS FUELS↗
DOE OSTI2025

Evaluating CO 2 -to-formic acid electrocatalysts in different device configurations

We evaluated CO 2 electroreduction differences of three materials in aqueous H-cell, gas diffusion electrode (GDE) half-cell, and full-cell electrolyzer devices. Mass-transport limited catalyst differences in H-cells become more apparent in gas-fed GDE half-cells; however, voltage contributions from device components can mask cathode differences in full-cell devices until high current density.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Hybrid Doping Strategy with High‐Entropy Cu/Fe Surface Modification and Zr Bulk Incorporation for Ni‐Rich Cathodes

A hybrid doping strategy combining Zr 4+ bulk doping with high-entropy Cu 2+ /Fe 3+ surface doping is developed to enhance the structural and interfacial stability of Ni-rich layered oxide cathodes. Cu and Fe are selectively introduced at the particle surface via a surface-selective ion-exchange process, forming a ≈15 nm Fe-rich layer while preserving the layered framework. Compared to the pristine cathode, the hybrid sample exhibits significantly improved electrochemical performance in both half-cell and full-cell configurations. In half-cells, the hybrid retains 88.5% and 90.2% after 100 cycles at 1C under 4.6 and 4.5 V, respectively. During high-voltage full-cell cycling, the hybrid cathode maintains over 80% capacity retention, whereas the pristine counterpart retains less than 10% under identical conditions over the same cycling period. XPS, EELS, and DEMS analyses confirm improved oxygen retention, suppressed gas evolution, and stable surface chemistry, while DFT calculations indicate enhanced Me–O bonding in the selected Fe 0.75 Cu 0.25 (Mn 1/16 Co 2/16 Ni 13/16 )O 2 surface composition, which is identified through DFT-calculated mixing energy reaching a minimum at this ratio, indicating the most thermodynamically favorable configuration. In conclusion, these results demonstrate the effectiveness of this hybrid doping strategy in mitigating coupled degradation pathways in Ni-rich cathodes.

15 GEOTHERMAL ENERGY↗
DOE OSTI2026

Binder-Stabilized Carbon Fiber Hosts for High-Utilization Sodium–Polysulfide Flow Catholytes

Sodium-sulfur (Na-S) batteries hold promise as high-energy-density batteries for long-duration energy storage due to their high open circuit voltage and Earth-abundant active materials. However, low utilization of the sulfur active material limits the achievable specific capacity, especially when a liquid polysulfide catholyte is utilized. High-surface-area carbon materials demonstrate promise to increase sulfur utilization in a Na-S battery. To make the carbon host material applicable for a flow battery application, a binder is required to bind the carbon materials together and to a porous substrate. Here, we utilize a composite carbon paper electrode coated by polymer,carbon nanofibers (CNFs) and carbon black (CB). By varying the mass ratios of CNF to CB, we found that a 70/20/10 mass ratio of CNF/CB/binder provided the highest capacity (260 mAh g −1 compared to the baseline of 156 mAh g −1 ) and stable battery performance over 100 cycles. Analysis of the composite electrode and full cells reveals that the amount of CB in the composite electrode influences binder distribution, cell resistance, and full cell performance.

Lehmann, Michelle L. [Oak Ridge National Laborator↗
DOE OSTI2021

Functionalized Embedded Monometallic Nickel Catalysts for Enhanced Hydrogen Evolution: Performance and Stability

Viable anionic exchange membrane (AEM) electrolysis for H 2 production requires highly active hydrogen evolution reaction (HER) catalysts that are also robust and cost-effective. Traditionally juxtaposition of two transition metals with one being more oxophilic is necessary for easier access to water in the inner Helmholtz plane as a source of protons in the crucial Volmer step for enhanced HER activity. However, they are prone to passivation at anodic potentials or deactivation via the formation of sub-surface metal hydrides at high cathodic overpotentials. Here we report a method of enabling close juxtaposition of Ni-Ni-oxide surfaces by functionalizing Ni-based catalysts via the careful thermal treatment of carbon-supported Ni nano-particles chelated with a select organic chelating compound referred to as cupferron. This functionalization results in an embedded Ni surface with a clear graphitic coating engendering long-term stability for passivation and subsurface hydride formation. The stability and activity of the functionalized Ni catalyst are demonstrated in half-cell RDE and full-cell AEM membrane-based hydrogen pump experiments. In the case of the latter, the functionalized Ni outperforms carbon-supported Pt.

25 ENERGY STORAGE↗
DOE OSTI2020

Enabling high areal capacity for Co-free high voltage spinel materials in next-generation Li-ion batteries

The rapidly growing technological demand for lithium-ion batteries has prompted the development of novel cathode materials with high energy density, low cost, and improved safety. High voltage spinel, LiNi 0.5 Mn 1.5 O 4 (LNMO), is one of the most promising candidates yet to be commercialized. The two primary obstacles for this material are the inferior electronic conductivity and fast capacity degradation in full cells due to the high operating voltage. By systematically addressing these limitations, we successfully develop a thick LNMO electrode with areal capacity loadings up to 3 mAh·cm –2 . The optimized thick electrode is paired with a commercial graphite anode at both the coin cell and pouch cell level, achieving a full cell capacity retention as high as 72% and 78%, respectively, after 300 cycles. We attribute this superior cycling stability to careful optimizations of cell components and testing conditions, with a specific focus improving electronic conductivity and high voltage compatibility. These results suggest precise control of materials quality, electrode architecture and electrolyte optimization can soon support the development of a cobalt-free battery system based on a thick LNMO cathode (>4 mAh·cm 2 ), which will eventually meet the needs of next-generation Li-ion batteries with reduced cost, improved safety, and assured sustainability.

25 ENERGY STORAGE↗
DOE OSTI2022

Mitigation of rapid capacity decay in silicon-LiNi 0.6 Mn 0.2 Co 0.2 O 2 full batteries

Silicon (Si)-based materials have been considered as the most promising anode materials for high-energy-density lithium-ion batteries because of their higher storage capacity and similar operating voltage, as compared to the commercial graphite (Gr) anode. But the use of Si anodes including silicon-graphite (Si-Gr) blended anodes often leads to rapid capacity decay in Si-Gr/LiNixMnyCo z O 2 (x+y+z=1) full cells, which has been attributed to surface instability of the Si component. In addition to stabilizing the surface, this work investigates the potential of the Si-Gr blended anodes in a full-cell configuration and its impact on the capacity contribution from active components. Using dQ/dV plots of the full cells, a powerful but simple-to-implement differential potential approach is developed to decouple the capacity contribution and degradation from the graphite and silicon components. Data collected from three-electrode cells confirm the results from the differential potential approach, which suggests a voltage slippage to a higher voltage at the blended anode side. Additionally, the voltage slippage causes a reduced utilization of the Gr component and exacerbates side reactions between the Si-Gr anode and carbonate electrolytes. Furthermore, based on these failure mechanisms, we adopted a mitigation strategy to tune the open circuit voltage of the prelithiated anode while stabilizing the surface. As a result, the full cells with the modified Si-Gr anodes (mass loading, 2.5 mAh/cm 2 ) offer a highly reversible full-cell energy density of 390 Wh/kg (based on the mass of both anode and cathode materials in a full cell) with a cycling CE of 99.9% over 200 cycles.

25 ENERGY STORAGE↗
DOE OSTI2025

Stable Cycling of Sodium All‐Solid‐State Batteries with High‐Capacity Cathode Presodiation

Sodium all-solid-state batteries (NaSSBs) with an alloy-type anode (e.g., Sn and Sb) offer superior capacity and energy density compared to hard carbon anode. However, the irreversible loss of Na + at the alloy anode during the initial cycle results in diminished capacity and stability, impairing full-cell performance. Here, this study presents an easy-to-implement cathode presodiation strategy by employing a Na-rich material to address these challenges. Leveraging the high theoretical capacity and suitable voltage window, Na 2 S is chosen as the Na donor, which is activated by creating a mixed electron-ion conducting network, delivering a high capacity of 511.7 mAh g −1 . By adding a small amount (i.e., 3 wt.%) of Na 2 S to the cathode composite, a NaCrO 2 || Sn full cell demonstrated capacity improvement from 90.8 to 118.2 mAh g −1 (based on cathode mass). The capacity-balanced full cell can thus cycle to more than 300 times with >90% capacity retention. This work provides a practical solution to enhance the full-cell performance and advance the transformation from half-cell to full-cell applications of NaSSBs.

25 - ENERGY STORAGE↗
DOE OSTI2022

Ultra-Stretchable, Ionic Conducting, Pressure-Sensitive Adhesive with Dual Role for Stable Li-Metal Batteries

The practical application of lithium (Li) metal battery is impeded by the Li dendrite growth and unstable solid electrolyte interphase (SEI) layer. Herein, an ultra-stretchable and ionic conducting chemically crosslinked pressure-sensitive adhesive (cPSA) synthesized via the copolymerization of 2-ethylhexyl acrylate and acrylic acid with poly(ethyleneglycol)dimethacrylate as crosslinker (short for 70cPSA), is developed as both artificial SEI layer and solid polymer electrolyte (SPE) for stable Li-metal electrode, enabling all-solid-state Li metal batteries with excellent cycling performance. As an artificial SEI layer, the 70cPSA-modified electrodes exhibit excellent electrochemical performance in Li|70cPSA@Cu half cells and 70cPSA@Li|70cPSA@Li symmetric cells. In full cells with LiFePO 4 (LFP) as cathode, the 70cPSA@Li|LFP cell exhibits stable cycling performance over 250 cycles. Utilized as SPE, the all-solid-state Li|SPE|LFP cell delivers excellent cycling stability with a capacity retention of 86% over 500 cycles. With high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) as cathode, the Li|SPE|NMC811 cell exhibits a discharge capacity of 124.3 mAh g -1 with a capacity retention of 71% after 200 cycles. Furthermore, the rational design of PSAs and investigation of their dual role for stable and safe Li-metal batteries may shed a light on adhesive polymers for battery applications.

25 ENERGY STORAGE↗
DOE OSTI2024

Lithicone‐Protected Lithium Metal Anodes for Lithium Metal Batteries with Nickel‐Rich Cathode Materials

The high energy density advantage of lithium (Li) metal batteries (LMBs) makes them increasingly desirable; however, problems such as strong reactivity and dendrite growth of Li metal anode limit their practical uses. In this work, a novel Li‐containing glycerol (LiGL) or lithicone protection layer on a 50 μm thick Li metal anode is employed for improving the performance of LMBs. This LiGL layer was accurately deposited via a molecular layer deposition (MLD) process at 150 °C, using lithium tert‐butoxide and glycerol as precursors. The as‐formed LiGL coating layer is highly tunable in its thickness by simply adjusting MLD cycles and shows a good stability and outstanding ionic transport properties. The LiGL layer is found to effectively mitigate side reactions and enhance cycling stability in both symmetric cells and full cells. Specifically, the LMBs with LiGL@Li anode of 400 MLD cycles and LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode enable a capacity retention of ≈87%, much higher than ≈35% of the cells with bare Li after 200 cycles at a charge/discharge current density of 2.1 mA cm −2 . This work paves a feasible way for practical LMBs with improved capacity and stability through applying an innovative protection layer on Li metal anodes.

25 ENERGY STORAGE↗
DOE OSTI2022

Recent progress in in-situ visualization of electrochemical reactions in electrochemical energy devices

A growing body of evidence indicates that bubble dynamics are crucial performance-limiting factors on electrochemical reactions and energy conversion efficiencies in both half-cell and full cell device levels. This review aims to summarize the recent progress in in-situ visualization characterizations of electrochemical reactions and reactant/product transport in electrochemical energy systems. The latest achievements of various new electrodes, transparent cell designs, and development for simultaneous visualization of reactions at both electrodes and electrolyte/electrode interface are highlighted. The new insights into the influence of bubbles on reaction sites and associated electrochemical performances are discussed. Lastly, some perspectives on potential strategies for mitigating the bubble-induced energy losses are proposed for future research directions and opportunities in water electrolysis and other electrochemical energy systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

In situ polymerized succinonitrile-based solid polymer electrolytes for lithium ion batteries

Novel solid polymer electrolytes based on succinonitrile (SN) plastic crystal electrolyte (SN-PCE) and polymerized ionic liquid (PIL) has been successfully synthesized via an in-situ method. The fabricated electrolyte (PIL-SN-PCE) is uniformly inlayed into the supporting matrix of polyimide, which effectively ameliorates the mechanical properties of the electrolyte. PIL can effectively enhance the thermal stability of electrolytes up to 300 °C and mitigate the parasitic reactions between the electrolytes and the electrodes. PIL-SN-PCE exhibits a remarkable oxidation ability up to 5.4 V vs Li/Li + and a high room temperature ionic conductivity of 6.54 × 10 -4 S cm -1 . Furthermore, in-situ formed interface in PIL-SN-PCE guarantee an excellent compatibility with different electrodes, which can effectively improve the cycle stability and rate performances of both half-cells and full cells. Finally, PIL-SN-PCE is considered as a promising electrolyte for high energy density lithium-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Surface and Bulk Stabilization of Silicon Anodes with Mixed-Multivalent Additives: Ca(TFSI) 2 and Mg(TFSI) 2

Here, silicon is drawing attention as the upcoming anode material for the next generation of lithium-ion batteries due to its higher capacity compared to commercial graphite. However, silicon anions formed during lithiation are highly reactive with binder and electrolyte components creating an unstable SEI layer and limiting the calendar life of silicon anodes. The reactivity of lithium silicide and the formation of an unstable SEI layer is mitigated by utilizing the use of a mixture of Ca and Mg multivalent cations as an electrolyte additive for Si anodes to improve their calendar life. The effect of mixed salts on the bulk and surface of silicon anodes was studied by multiple structural characterization techniques. Ca and Mg ions in the electrolyte formed relatively thermodynamically stable quaternary Li-Ca-Mg-Si Zintl phases in an in-situ fashion and more stable and denser SEI layer on the Si particles. These in turn protect silicon particles against side reactions with electrolytes in a coin cell. The full cell with the mixed cation electrolyte demonstrates enhanced calendar life performance with lower measured current and current leakage than that of the baseline electrolyte due to reduced side reactions. Electron Microscopy, HRXRD, and solid-state NMR results showed that electrodes with mixed cations tended to have less cracking on the electrode surface compared to Si electrodes with Gen2 + FEC and the presence of mixed cations enhances cation migration and formation of quaternary Zintl phases stabilizing bulk and forming a more stable SEI.

25 ENERGY STORAGE↗
DOE OSTI2025

Highly textured metal anodes for stable aqueous batteries: Fabrication and characterization

We report a purely mechanical “cold-compression flow” method for fabricating Zn, Sn, and In substrates with tunable crystallographic textures. Using textured Zn as a model system, we investigate Zn electrocrystallization and demonstrate correlated growth of crystalline films with correlation lengths from tens to hundreds of micrometers. At 5 milliamperes per square centimeter (mA/cm 2 ), capacities between 20 and 82 milliampere hours per square centimeter (mA·hour/cm 2 ) are achieved depending on substrate texture level. At higher currents (40 mA/cm 2 ), capacities reach up to 604 mA·hour/cm 2 . Rotating disk electrode studies show that dominantly (002) textured Zn substrates exhibit enhanced corrosion resistance and reduced interphase passivation. We introduce an effective Damköhler number (Da*) to concisely describe morphological evolution during electrocrystallization across substrates with different textures. High-texture (002) Zn substrates substantially enhance performance in high-capacity (~20 mA·hour/cm 2 ) symmetric Zn||Zn cells and full cells (Zn||δ-MnO 2 and Zn||I 2 ), enabling fast-charging and prolonged energy storage in coin and pouch rechargeable Zn battery formats.

Science & Technology - Other Topics↗
DOE OSTI2025

Demonstration of MgCr 2– x Mn x O 4 Spinel Oxide Cathodes in High-Voltage Mg Batteries

Solid-solution oxide spinels with high redox voltages and facile Mg 2+ mobility have been identified as promising candidates for practical, high-voltage cathodes in Mg batteries. In this work, we discuss the development of MgCr 2-x Mn x O 4 [x = 0.5, 1, 1.2] solid-solution spinel oxides as a cathode material and their electrochemical performance paired with an Mg anode in a full cell. This work presents the first demonstration of full cells with these materials. Mg-Cr-Mn spinel oxides with varying Cr and Mn contents were synthesized using alternative synthetic routes for optimal electrochemical performance. High-resolution synchrotron powder X-ray diffraction (PXRD), solid-state nuclear magnetic resonance (NMR) spectroscopy, and electron microscopy showed that these different synthetic routes resulted in changes in structures and particle morphologies, which in turn affect the electrochemical performance. Particularly, the urea coprecipitation synthetic route resulted in high-surface-area particles that enabled lower overpotentials and increased discharge capacity. The high surface area also resulted in expedited structural degradation caused by the irreversible migration of Mg 2+ into normally vacant 16c sites in the spinel lattice. This structural degradation was lessened by using a hydrosauna-urea synthesis method, which decreased the Mg/Mn inversion ratio while retaining high-surface-area particles with good cycling performance. Furthermore, our findings highlight the necessity for high surface area or nanostructured spinel oxide cathodes with minimized Mg-Mn inversion to enable spinel oxide cathodes in Mg full cells.

Mg anode↗
DOE OSTI2026

All-organic self-separating three-dimensionally nanoarchitected electrochemical energy storage devices

This work realizes a three-dimensionally (3D) nanoarchitected, all organic, "self-separating" lithium-ion electrochemical energy storage (EES) device that is cycled as a solid-state full cell. The device is enabled by a monolithic carbon anode with a co-continuous pore network, derived from the structure direction of resols by an ultra-large molar mass block copolymer (BCP), poly(styrene-block-2-dimethylaminoethyl methacrylate) (SA). Electropolymerization of a single-phase conductive and redox-active material, poly((2,3-dihydrothieno[3,4-b][1,4]dioxin-2-yl)methyl 9,10-dioxo-9,10-dihydroanthracene-2-carboxylate) (PAQEDOT), into the pore space provides the cathode of the cell. The device is electronically contacted to the relevant electrode network enabled by the co-continuous nature of each electrode. Electrochemical processing via cycling against external lithium in an electrolyte generates a solid electrolyte interphase (SEI) as a separator and lithiates the cell electrodes, after which the EES device is cycled in the solid state. While the full cell does not demonstrate high cyclability, the best full cell demonstrates a discharge capacity of 267 milliamp hours per gram (mAh/g). This work marks, to the best of knowledge of the authors, the first example of an all-organic materials derived 3D nanoarchitected EES device, as well as the first design of "self-separating" cell fabrication. Furthermore, generalization of the design to another co-continuous carbon form factor is demonstrated.

FOS: Physical sciences↗