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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

Cycling Performance and Structure Evolution of Co-Free Lithium- and Manganese-Rich Layered Oxides in Lithium-Ion Batteries

Lithium- and manganese-rich (LMR) layered oxides are high-capacity cathode materials that are being considered for electric vehicle (EV) lithium-ion batteries (LIBs). Here, we investigate the electrochemical cycling behavior of cells containing a cobalt-free LMR oxide, 0.3Li 2 MnO 3 ·0.7LiMn 0.5 Ni 0.5 O 2 , paired with either Li or graphite anodes. Two- and three-electrode cells are cycled under varying conditions to examine the effects of oxide activation, upper cutoff voltage, separator type, and electrolyte composition. Post-cycling characterization of harvested electrodes, with electrochemical, X-ray absorption spectroscopy, and solid-state 6 Li nuclear magnetic resonance spectroscopy techniques, are used to correlate cell performance changes with redox state evolution in the oxide and Li inventory shifts in the cell. Our results show that capacity fade and impedance rise primarily originate at the graphite anode and LMR cathode, respectively. Notably, while Ni undergoes reversible redox, Mn shows no evidence of bulk redox activity even in highly-aged electrodes: only relithiated LMR electrodes show some reduction of Mn. Graphite electrodes degrade due to particle isolation and SEI growth, exacerbated by Mn dissolution and deposition on graphite anodes. These findings highlight the coupled structural and electrochemical degradation mechanisms in LMR/graphite cells and underscore lithium inventory retention and electrode interfacial stability as critical factors for enhancing long-term performance.

Badami, Pavan P. [Argonne National Laboratory (ANL↗
DOE OSTI2026

Performance Enhancement of the Transcritical CO2 Cycle with a Near-Isothermal Liquid Piston Compression by an Ejector

This study investigates the use of an ejector in a transcritical CO2 cycle employing a near-isothermal liquid piston compressor, with the objective of mitigating refrigerant degassing in mineral oil. While the liquid piston compressor demonstrated high isothermal efficiency (˜90%), overall cycle performance was limited by CO2 degassing during chamber pressure fluctuations. A thermodynamic model was developed to compare baseline and ejector-assisted cycles, incorporating solubility correlations, entrainment ratio characteristics, and a degassing correction factor. Results indicate that the ejector increased suction pressure and reduced CO2–oil solubility variation, which improved refrigerant intake and reduced degassing losses. Despite these benefits, the ejector-assisted cycle showed a lower coefficient of performance (COP) than the baseline. Possible contributing factors include the limited marginal benefit of pressure reduction in a highly efficient isothermal compressor, reduced effectiveness of the separator due to the use of a suction-line heat exchanger in both cycles, and uncertainties in the solubility data under transient conditions. These findings suggest that degassing mitigation is essential for realizing the potential of liquid piston compression, but ejector integration alone is unlikely to enhance COP. Future work should focus on ejector optimization, improved oil–refrigerant management, introducing less-soluble working liquids, and experimental validation under realistic operating conditions.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2026

Mechanistic Understanding of Interphase-driven Aging in Silicon Anodes

Conventional solid electrolyte interphases (SEIs) strongly adhere to micro-silicon (µ-Si) and crack under volume changes, causing poor cycling performance. Nano-silicon improves cycling performance but remains costly with limited calendar life. Here potentiostatic ageing tests demonstrate that both calendar and cycle ageing are governed by SEI cracking and dissolution with different relative contributions. When the system is not dominated by SEI dissolution, the relative calendar life of Si anodes could correlates positively with their cycle life. LiF-rich SEI that enables long cycle life in µ-Si is therefore expected to enhance calendar life as well. Using this framework, we screened electrolytes, SEIs and electrodes and validated them with full-cell storage. LiF-rich SEI minimizes cracking and dissolution, enabling μ-Si to achieve excellent calendar life, whereas nano-silicon suffers from SEI dissolution and needs reduced electrolyte–electrode contact for better calendar life. This work clarifies calendar-ageing behaviour and accelerates electrolytes and SEI development for long-life Si anodes.

Johnson, Christopher S.↗
DOE OSTI2024

Crack‐Free Single‐Crystalline LiNiO 2 for High Energy Density All‐Solid‐State Batteries

Abstract Single‐crystalline layered oxide (LiNi 1‐ x ‐ y Mn x Co y O 2 ) cathodes have been found to exhibit exceptional electrochemical properties when coupled with various inorganic solid electrolytes (ISEs) in all‐solid‐state batteries (ASSBs). Their advantages stem from the robust morphological integrity with the absence of grain boundaries and the high electrochemical oxidative stability. Here, ASSBs featuring single‐crystalline LiNiO 2 (LNO) with the highest Ni content are reported, offering a high theoretical specific capacity of 275 mAh g ‐1 alongside a high average discharge voltage (3.7 V vs Li + /Li). Through a careful investigation, it is demonstrated that micron‐sized single‐crystalline LNO (µSC‐LNO) composite cathodes with a halide ISE exhibit a high initial discharge capacity of 205 mAh g ‐1 with an outstanding cycle performance over 200 cycles in room‐temperature ASSBs. The significance of engineering parameters is emphasized, such as particle size and specific density, in promoting a homogeneous and fast Li + transport within the composite cathodes. Furthermore, the formation of undesirable interphase between the halide ISE in the cathode and sulfide ISE separator is elucidated, which may be a critical factor impeding long‐term cyclability of ASSBs. This work provides insights into the design of composite cathodes for high‐energy‐density ASSBs.

Chemistry↗
DOE OSTI2025

Investigating the effect of screen-printed structured graphite electrodes with low tortuosity for high-capacity and fast-charging lithium-ion batteries

A flexible screen-printed graphite electrode was fabricated as an anode for developing fast-charging lithium-ion batteries with low tortuosity. A homogenous anode ink was prepared by mixing graphite as the active material, carbon black (C45) as the conductive additive, and polyvinylidene fluoride (PVDF) as the binder in N-Methyl-2-pyrrolidone (NMP) solvent. The ink was deposited on a flexible copper foil via a stainless-steel screen consisting of an array of pores, that act as secondary pore networks (SPNs), using the screen-printing process. Lithium-ion battery half-cells were assembled using the printed graphite anode, lithium metal foil as the counter electrode, and 1.2 M lithium hexafluorophosphate (LiPF 6 ) in ethyl carbonate: ethyl methyl carbonate (EC: EMC = 3:7) as the electrolyte. The effect of SPNs on the cell performance was investigated by performing formation, rate and cycling tests on the assembled cells, at different C-rates. It was observed that the cells consisting of SPNs with a pore size of 100 μm and edge-to-edge distance of 100 μm between the pores exhibited significantly higher specific capacities of 168 and 129 mAh/g when compared to reference cells without SPNs, which had capacities of 120 and 85 mAh/g, at high C-rates of 4 C and 6 C, respectively. The cells with SPNs also demonstrated excellent cycling performance with ~ 95% capacity retention after 100 cycles at 2 C.

Fast charging lithium-ion battery↗
DOE OSTI2024

Structure–performance relationships of lithium-ion battery cathodes revealed by contrast-variation small-angle neutron scattering

Lithium-ion battery cathodes are porous composites of active material, conductive carbon, and polymer binder. Controlling the cathode microstructure is key to achieving high energy density and cycling stability. Current characterization techniques lack the nanoscale resolution over representative volumes necessary to relate cathode microstructure to cycling performance. To address this challenge, we utilize contrast-variation small-angle neutron scattering to quantify the chemical and structural features of cathodes wet by dimethyl carbonate, representing a relevant solvent environment. Using neutron scattering measurements, we identify an expansion in carbon and polymer structures that arises after calendering and wetting with solvent. Further, we deconvolute the carbon and binder phases to obtain the solvent-accessible carbon black surface area, which we correlate to diminished capacity retention driven by electrolyte decomposition on exposed carbon. This technique provides nanoscale insight into composite cathode microstructures and resulting cycling performance, promising future applications to a broad range of porous materials that exist in energy storage systems.

25 ENERGY STORAGE↗
DOE OSTI2025

Interphase Engineering Enabled by Using a Separator with Electrochemically Active Carbazole Polymers for Lithium-Ion Batteries

Separators are generally considered inert components in lithium-ion batteries. In the past, some electroactive polymers have been successfully applied in separator modifications for overcharge protection or as acid scavengers. This study highlights the first use of two “electroactive” carbazole polymers (copolymer 9-phenyl-9H-carbazole-phenyl [PCP] and poly(9-vinylcarbazole) [PVC]), which were each applied separately as coatings on the cathode-facing side of commercial Celgard 2325 separators, respectively, to enhance the cycling performance of 0.3Li 2 MnO 3 ·0.7LiMn 0.5 Ni 0.5 O 2 //graphite (LMR-NM//Gr) full cells through interphase engineering. The team observed an irreversible polymer oxidation process of the carbazole-functionalized polymers—occurring only during the first charge—for the modified separator cells, and the results were confirmed by dQ/dV analysis, cyclic voltammetry measurements, and nuclear magnetic resonance characterizations. During this oxidation, carbazole polymers participate in the process of interphase formation, contributing to the improved cycling performance of LMR-NM//Gr batteries. Particularly, oxidation takes place at voltages of ~4.0 and ~3.5 V when PCP and PVC are used as separator coatings, which is highly irreversible. Further postmortem examinations suggest that the improvements using these modified separators arise from the formation of higher-quality and more inorganic SEI, as well as the beneficial CEI enriched in LixPOyFz. These interphases effectively inhibit the crosstalk effect by reducing TM dissolution.

carbazole↗
DOE OSTI2025

Direct Prelithiation of Silicon-Based Composite Electrodes via Island-like Thermal Evaporation

Irreversible losses of Li during solid electrolyte interface (SEI) conditioning is a key contributor to the lower specific capacities observed in silicon-containing Li-ion batteries. Herein, thermal evaporation of between 1 and 20 µm of Li onto Si-based composite anodes has been investigated as a prelithiation method to account for such losses. To account for mechanical strain caused by Li-Si alloying during the deposition, a stainless-steel mesh is applied to the electrodes before prelithiation to form “island-like” deposition on the electrode surface. The open circuit potential was also found to decrease as a function of increased Li evaporation, consistent with the potentials of electrochemically prepared LixSi alloys. Prelithiating to account for irreversible Li losses to SEI formation resulted in full cells with a 15.8% increase in initial coulombic efficiency and a 47.8% reduction in irreversible capacity loss after SEI formation cycling. Subsequent C/3 cycling showed up to a 62.9% increase in specific capacity in prelithiated cells. X-ray photoelectron spectroscopy (XPS) revealed differences in the SEI composition that was formed by electrochemical cycling and reactively formed in prelithiated cells upon exposure to Gen2 + 3% FEC electrolyte. The reactively formed SEI from the spontaneous reaction with lithiated silicon was carbonate-rich while the electrochemical SEI formation showed significantly more LiPFx species, which could play a role in overall cycling performance.

Musgrove, Amanda↗
DOE OSTI2024

The Impact of Lithium Anode Interface on Capacity Fade in Polymer Electrolyte-Based Solid-State Batteries

This study investigates the Li stripping-plating morphology and failure mechanisms in full cells consisting of a solid polymer electrolyte (SPE) with two commercial Li anodes: Li chip and Li foil. The primary identified failure mechanism of the SPE cell is capacity fade, regardless of the Li manufacturer. While the cathode’s role in capacity fade is evident, the Li anode significantly influences cycling performance, with Li foil cells cycling 50% longer than Li chip cells, a statistical difference. Further, post-mortem scanning electron microscopy and X-ray photoelectron spectroscopy results attribute the Li chip’s faster capacity fade to a loss of contact and continuous growth of the solid electrolyte interphase (SEI). Conversely, Li foil maintains consistent contact with the solid polymer, displaying a thin and stable SEI. Additionally, failure mechanisms between a gel electrolyte in previous work and the dry SPE are compared.

25 ENERGY STORAGE↗
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 OSTI2024

New Thermochemical Salt Hydrate System for Energy Storage in Buildings

This paper introduces an innovative design for an “inorganic salt-expanded graphite” composite thermochemical system. The storage unit is made of a perforated, compressed, expanded graphite block impregnated with molten CaCl 2 ∙6H 2 O; the humid air passes through the holes that allow the moisture to diffuse and react with the salt. The prepared block underwent 90 hydration-dehydration cycles. Although most of the performed cycles were carried out with salt overhydration and deliquescence, the treated samples have remained mechanically and thermally stable with no drop in energy density. The volumetric energy density of the composite ranged from 135.5 to 277.6 kWh/m 3 , depending on airflow rate and absolute humidity. To ensure composite material cycling stability, the energy density of the block was measured during hydration at similar conditions of absolute humidity, inlet temperature, and airflow rate (0.01 kg water /kg air , 20 °C, 400 l/min). The average energy density at these conditions was sustained at 219 kWh/m 3 . The block integrity was monitored by visual inspection after removing it from the reactor chamber every few cycles. Both the composite material and its manufacturing process are simple and easy to scale up for future commercialization.

25 ENERGY STORAGE↗
DOE OSTI2024

Quantitative Identification of Dopant Occupation in Li‐Rich Cathodes

Elemental doping is widely used to improve the performance of cathode materials in lithium‐ion batteries. However, macroscopic/statistical investigation on how doping sites are distributed in the material lattice, despite being a key prerequisite for understanding and manipulating the doping effect, has not been effectively established. Herein, to solve this predicament, a universal strategy is proposed to quantitatively identify the locations of Al and Mg dopants in lithium‐rich layered oxides (LLOs). Solid evidence confirms that Al prefers to occupy the transition metal (TM) layer, while Mg evenly occupies both TM and Li layers. As a result, Mg significantly reduces the thickness of LiO 2 slabs at room temperature, which will increase the energy barrier of oxygen activation and enhance the structure stability of LLOs. The suppressed oxygen activity in Mg‐doped LLO can be kinetically unlocked at 55 °C. The different characteristics of Al and Mg enlighten an Al/Mg co‐doping strategy to optimize LLOs, which significantly improves the cycle performance while lifting the capacity. In conclusion, these insights from the quantitative identification of doping sites shed light on the manipulation of doping effects toward better cathodes.

25 ENERGY STORAGE↗
DOE OSTI2025

Design of Sodium Chalcohalide Solid Electrolytes with Mixed Anions for All‐Solid‐State Sodium‐Ion Batteries

Solid-state sodium-ion batteries (SSNIBs) have emerged as a promising alternative to lithium-ion systems for grid-scale energy storage, owing to sodium's abundance and the improved safety of solid-state designs. Among various solid-state electrolytes (SSEs), halide-based Na + SSEs offer high electrochemical stability but are limited by low ionic conductivity and poor thermal stability. Herein, a novel class of sodium hafnium chalcohalide SSEs is reported with a dual-anion (S 2− /Cl − ) framework, with a high ionic conductivity of 4.5 × 10 −4 S cm −1 . The incorporation of sulfur enhances Na⁺ mobility by reducing the migration barrier through increased anion polarizability and expanded diffusion pathways. Additionally, S 2− contributes to stronger interatomic bonding, leading to higher cohesive energy density, improved thermal stability, and mechanical robustness. These SSEs exhibit minimal sulfur oxidation and excellent chemical/electrochemical interface stability with different cathode materials, such as O3-layered NaNi 1/3 Fe 1/3 Mn 1/3 O 2 , P2/O3 layered Na 0.85 Mn 0.5 Ni 0.4 Fe 0.1 O 2 , and Na 3 V 2 (PO 4 ) 3 cathodes. As a result, SSNIBs with P2/O3 layered Na 0.85 Mn 0.5 Ni 0.4 Fe 0.1 O 2 employing the sodium hafnium chalcohalide SSEs demonstrate outstanding cycling performance, achieving a capacity retention of 88.5% after 200 cycles at 0.1 C. This study establishes a new design strategy for high-performance SSEs, demonstrating that mixed-anion frameworks offer a viable route to overcome the intrinsic limitations of single-anion electrolytes in next-generation SSNIBs.

DFT calculation↗
DOE OSTI2026

Reducing Internal Resistance in Activated Carbon Supercapacitors via Exfoliated Coal-Derived Graphene Additive

Low equivalent series resistance (ESR) is critical for high-rate energy storage devices (e.g., supercapacitors), and graphene is a promising additive for reducing ESR in carbon-based supercapacitor electrodes. However, graphene can be costly and difficult to produce at scale. This study investigates the addition of graphene, produced through electrochemical exfoliation of domestic coal-derived graphite, in activated carbon-based supercapacitors. The coal-derived graphene was incorporated at varying weight loadings and tested in symmetric supercapacitors with aqueous electrolytes. ESR was evaluated using both direct current internal resistance (DCIR) and electrochemical impedance spectroscopy (EIS) measurements. DCIR measurements revealed ESR reductions of ∼34%, ∼18%, and ∼21% at 3, 5, and 10 wt % loadings, respectively, compared to the baseline (0 wt %) of ∼0.54 Ω. These results were further confirmed by EIS measurements. Correspondingly, power density increased by ∼52%, ∼27%, and ∼35% at 3, 5, and 10 wt % loadings relative to the baseline (∼29 kW/kg). Additionally, the electrodes exhibited moderate increases in specific capacitance and energy density, along with stable cycling performance (capacitance retention above 85% after 100,000 cycles) and capacitive behavior (α = 0.95−0.97), suggesting favorable charge transfer kinetics. These findings highlight the potential of exfoliated coal-derived graphene as an effective additive for supercapacitor electrodes.

capacitors↗
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 OSTI2024

Self‐Templated 3D Sulfide‐Based Solid Composite Electrolyte for Solid‐State Sodium Metal Batteries

Abstract Rechargeable solid‐state sodium metal batteries (SSMBs) experience growing attention owing to the increased energy density (vs Na‐ion batteries) and cost‐effective materials. Inorganic sulfide‐based Na‐ion conductors also possess significant potential as promising solid electrolytes (SEs) in SSMBs. Nevertheless, due to the highly reactive Na metal, poor interface compatibility is the biggest obstacle for inorganic sulfide solid electrolytes such as Na 3 SbS 4 to achieve high performance in SSMBs. To address such electrochemical instability at the interface, new design of sulfide SE nanostructures and interface engineering are highly essential. In this work, a facile and straightforward approach is reported to prepare 3D sulfide‐based solid composite electrolytes (SCEs), which utilize porous Na 3 SbS 4 (NSS) as a self‐templated framework and fill with a phase transition polymer. The 3D structured SCEs display obviously improved interface stability toward Na metal than pristine sulfide. The assembled SSMBs (with TiS 2 or FeS 2 as cathodes) deliver outstanding electrochemical cycling performance. Moreover, the cycling of high‐voltage oxide cathode Na 0.67 Ni 0.33 Mn 0.67 O 2 (NNMO) is also demonstrated in SSMBs using 3D sulfide‐based SCEs. This study presents a novel design on the self‐templated nanostructure of SCEs, paving the way for the advancement of high‐energy sodium metal batteries.

Guo, Xiaolin↗
DOE OSTI2025

Asymmetric ether solvents for high-rate lithium metal batteries

Recent electrolyte solvent design based on weakening lithium-ion solvation have shown promise in enhancing cycling performance of Li-metal batteries. However, they often face slow redox kinetics and poor cycling reversibility at high rate. Here we report using asymmetric solvent molecules substantially accelerates Li redox kinetics. Asymmetric ethers (1-ethoxy-2-methoxyethane, 1-methoxy-2-propoxyethane) showed higher exchange current densities and enhanced high-rate Li 0 plating/stripping reversibility compared to symmetric ethers. Adjusting fluorination levels further improved oxidative stability and Li 0 reversibility. The asymmetric 1-(2,2,2-trifluoro)-ethoxy-2-methoxyethane, with 2 M lithium bis(fluorosulfonyl)imide, exhibited high exchange current density, oxidative stability, compact solid–electrolyte interphase (~10 nm). This electrolyte exhibited superior performance among state-of-the-art electrolytes, enabling over 220 cycles in high-rate Li (50 μm)||LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811, 4.9 mAh cm −2 ) cells and for the first time over 600 cycles in anode-free Cu | |Ni95 pouch cells (200 mAh) under electric vertical take-off and landing cycling protocols. Our findings on asymmetric molecular design strategy points to a new pathway towards achieving fast redox kinetics for high-power Li-metal batteries.

batteries↗