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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 1,477 records · Page 82
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Evaluating silicene as a potential cathode host to immobilize polysulfides in lithium–sulfur batteries

The internal shuttle effect caused by polysulfides dissolution and migration negatively impacts lithium–sulfur battery performance. In this paper, a mesoscale simulation strategy, which involves atomistic calculation and coarse-grained molecular modeling, is employed to evaluate silicene as a potential cathode host material to immobilize polysulfides. Adsorption energies of insoluble polysulfides (Li 2 S x with x =1, 2) and soluble polysulfide Li 2 S 4 on pristine and doped silicene sheets are calculated. Results show that the adsorption is thermodynamically favorable and N-doped silicene is helpful in trapping intermediate discharge products, Li 2 S 2 and Li 2 S 4 . The dissociation and reduction of long-chain polysulfides to short-chain polysulfides are observed. Electronic structure analysis shows that Li 2 S x molecules interact with silicene via strong chemical bonds. The atomistic structure evolution of Li 2 S layer formation on silicene is also investigated in this study. It is found that Li 2 S (110) layer forms first, and then, it is converted to Li 2 S (111) layer by introducing more Li 2 S molecules to the substrate. Li 2 S (111)/silicene interfacial structure is thermodynamically stable, and the interaction is dominated by Li–Si bonds. A coarse-grained model is developed to study and compare the growth of Li 2 S on silicene and graphene. Lastly, Li 2 S-induced surface coverage is faster on silicene than on graphene, which indicates that a silicene-based cathode host will experience more acute surface passivation, which will adversely affect cathode performance.

25 ENERGY STORAGE↗
DOE OSTI2019

Using in situ and operando methods to characterize phase changes in charged lithium nickel cobalt aluminum oxide cathode materials

Lithium ion batteries have been extensively explored in recent decades in order to improve their electrochemical performance, address safety concerns, and reduce costs in larger-scale applications. Electrode materials are key components which govern the properties of the battery at the system level. Cathode materials are of particular importance as they are a limiting factor for achieving high energy density. Lithium nickel cobalt aluminum oxide (LiNi 0.8 Co 0.15 Al 0.05 O 2 , referred to subsequently as NCA) is one of successful cathode materials since it can deliver higher capacity than other cathode materials such as lithium cobalt oxide or lithium iron phosphate. However, structural instabilities that occur NCA during charging or at high temperatures is believed to be the primary reason for performance degradation as well as a possible safety threat. Furthermore, understanding the structural evolution that occurs in NCA is of importance to acquire fundamental insights for taking full advantage of the high capacity of NCA materials. Beyond static information, in situ and operando characterization approaches allow us to observe structural changes under external stimulus or in a working condition, providing a deeper understanding of the routes by which structure evolve. In this review, we will describe the use of both in situ and operando characterization performed with both synchrotron X-ray based techniques and advanced electron microscopy, as the combination of these techniques have been shown to be particularly effective at providing structural information at complementary length scales.

25 ENERGY STORAGE↗
DOE OSTI2020

Quantifying redox heterogeneity in single-crystalline LiCoO 2 cathode particles

Active cathode particles are fundamental architectural units for the composite electrode of Li-ion batteries. The microstructure of the particles has a profound impact on their behavior and, consequently, on the cell-level electrochemical performance. LiCoO 2 (LCO, a dominant cathode material) is often in the form of well-shaped particles, a few micrometres in size, with good crystallinity. In contrast to secondary particles (an agglomeration of many fine primary grains), which are the other common form of battery particles populated with structural and chemical defects, it is often anticipated that good particle crystallinity leads to superior mechanical robustness and suppressed charge heterogeneity. Yet, sub-particle level charge inhomogeneity in LCO particles has been widely reported in the literature, posing a frontier challenge in this field. Herein, this topic is revisited and it is demonstrated that X-ray absorption spectra on single-crystalline particles with highly anisotropic lattice structures are sensitive to the polarization configuration of the incident X-rays, causing some degree of ambiguity in analyzing the local spectroscopic fingerprint. To tackle this issue, a methodology is developed that extracts the white-line peak energy in the X-ray absorption near-edge structure spectra as a key data attribute for representing the local state of charge in the LCO crystal. This method demonstrates significantly improved accuracy and reveals the mesoscale chemical complexity in LCO particles with better fidelity. In addition to the implications on the importance of particle engineering for LCO cathodes, the method developed herein also has significant impact on spectro-microscopic studies of single-crystalline materials at synchrotron facilities, which is broadly applicable to a wide range of scientific disciplines well beyond battery research.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Development of a 2 ns duration high current electron beam source using CsI coated carbon fibre cathode

A 50 ampere beam current having a rise time lesser than 500 pico-seconds with its energy 50 keV is generated using field emission mechanism. Beam duration was 2 ns. CsI coating on carbon fibre cathode was done using plasma spray coating. The results obtained from this cathode were compared to the carbon fibre cathode and the reason behind higher current density in the case of CsI coating has been explained. (author)

43 PARTICLE ACCELERATORS↗
DOE OSTI2016

Stability and Activity of (Pr 1‐x Nd x ) 2 NiO 4 as Cathodes for Solid Oxide Fuel Cells: I. Quantification of Phase Evolution in Pr 2 NiO 4

Praseodymium nickelate (Pr 2 NiO 4 ) is an active oxygen electrode for solid oxide fuel cells, but undergoes phase transition at elevated temperatures (e.g., 750°C). Quantification of this phase evolution in an operating single cell is challenging because of the overlap of X‐ray diffraction ( XRD ) peaks between the cathode and oxide current collector. In this work, we replace the oxide current collector with a gold metal grid, circumventing these challenges by allowing the exposure of the cathode to the X‐ray beam, while eliminating peak overlap. Quantification of the phase evolution was performed by a least‐squares fitting of the linear combination of XRD standards against the experimental patterns. Energy‐dispersive spectroscopy analysis on long‐term operated cells showed the absence of reactions between the gold grids and the cathodes. Additionally, the grids exhibited excellent mechanical stability under operating conditions and enabled similar cell performance as an oxide current collector.

Dogdibegovic, Emir↗
DOE OSTI2025

Unravelling electro-chemo-mechanical interplay in layered oxide cathode degradation in solid-state batteries

Solid-state batteries (SSBs) hold notable promise for advancing energy storage technologies. However, their commercial viability is limited by the poor cycle stability and complex degradation mechanism. This study underscores the pivotal role of electro-chemo-mechanical interactions in driving the failure of SSBs. Leveraging advanced x-ray imaging and spectroscopy techniques, we analyzed LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes from cycled Li x In||Li 6 PS 5 Cl (LPSC)||NMC811 SSBs, uncovering the interplay between microstructure, chemical heterogeneity, mechanical characteristics, and electrochemical performance. Our results show that revealing electro-chemo-mechanical interactions is essential to develop strategies to suppress the degradation of SSBs. Particularly, we revisit a LiNbO 3 (LNO) coating layer to mitigate electrochemical degradation. The LNO@NMC811 cathode retains 116 milliampere-hours per gram after 200 cycles, showing excellent stability, while the uncoated NMC811 cathode keeps degrading over time, with suppressed chemical heterogeneity and mechanical failure. This work highlights the importance of synergizing advanced material design with coating techniques, ensuring uniform lithium flux and improving mechanical properties to achieve stable, high-performance SSBs.

Zheng, Xueli [SLAC National Accelerator Laboratory↗
DOE OSTI2024

Unrecoverable lattice rotation governs structural degradation of single-crystalline cathodes

Transitioning from polycrystalline to single-crystalline nickel-rich cathodes has garnered considerable attention in both academia and industry, driven by advantages of high tap density and enhanced mechanical properties. However, cathodes with high nickel content (>70%) suffer from substantial capacity degradation, which poses a challenge to their commercial viability. Here, leveraging multiscale spatial resolution diffraction and imaging techniques, we observe that lattice rotations occur universally in single-crystalline cathodes and play a pivotal role in the structure degradation. These lattice rotations prove unrecoverable and govern the accumulation of adverse lattice distortions over repeated cycles, contributing to structural and mechanical degradation and fast capacity fade. These findings bridge the previous knowledge gap that exists in the mechanistic link between fast performance failure and atomic-scale structure degradation.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Structural Reliability of Cathode Contact Materials in Planar SOFCs

Despite significant developments in material and stack design technologies to enhance performance, the long-term mechanical reliability of solid oxide fuel cells remained an issue. The contact between electrodes and interconnects (especially the cathode side) was identified as one of the weakest links in present generation planar solid oxide fuel cells. Computational modeling was used to gain valuable insights on the cathode contact sintering mechanics and bond reliability. A continuum viscous sintering model was incorporated into a commercial finite element analysis code to simulate contact material densification and evaluate the bond and stack mechanical reliability due to developed stresses from the contact layer sintering. The parameters required for the cathode contact material constitutive model were extracted from experiments conducted for the contact material development at PNNL. The effects of contact layer thickness and sintering conditions like temperature and pressure on the stack stresses and reliability were investigated.

SOFC, FEA, Reliability↗
DOE OSTI2020

A Thermodynamic Reassessment of Lithium-Ion Battery Cathode Calorimetry

This work demonstrates how staged heat release from layered metal oxide cathodes in the presence of organic electrolytes can be predicted from basic thermodynamic properties. These prediction methods for heat release are an advancement compared to typical modeling approaches for thermal runaway in lithium-ion batteries, which tend to rely exclusively on calorimetry measurements of battery components. These calculations generate useful new insights when compared to calorimetry measurements for lithium cobalt oxide (LCO) as well as the most common varieties of nickel manganese cobalt oxide (NMC) and nickel cobalt aluminum oxide (NCA). Accurate trends in heat release with varying state of charge are predicted for all of these cathode materials. These results suggest that thermodynamic calculations utilizing a recently published database of properties are broadly applicable for predicting decomposition behavior of layered metal oxide cathodes. Aspects of literature calorimetry measurements relevant to thermal runaway modeling are identified and classified as thermodynamic or kinetic effects. The calorimetry measurements reviewed in this work will be useful for development of a new generation of thermal runaway models targeting applications where accurate maximum cell temperatures are required to predict cascading cell-to-cell propagation rates.

25 ENERGY STORAGE↗
DOE OSTI2021

Critical Barriers to Successful Implementation of Earth-Abundant, Mn-Rich Cathodes for Vehicle Applications and Beyond: A Detailed Study of Low SOC Impedance

We report that earth-abundant, sustainable cathode chemistries based on Mn are increasingly attractive for enabling a broader portfolio of cathode oxides. The well-known class of lithium- and manganese-rich cathodes still represents very viable options. However, despite the important work on understanding the mechanisms of voltage fade, hysteresis, and oxygen activity, relatively little attention has been given to understanding the impedance characteristics of these electrodes. In particular, an anomalous rise in area specific impedance at lower states of charge, as well as overall impedance rise and surface damage due to electrolyte interactions, represent critical barriers to implementation. This work presents a comprehensive study of impedance behavior in cobalt-free, lithium- and manganese-rich electrodes. The use of a robust surface treatment allows for long-term behavior to be probed in the absence of surface damage, capacity loss, and impedance rise due to electrolyte interactions. The anomalous rise in impedance could not be correlated to surface changes, or surface phase formation, but could be directly correlated with the bulk processes of voltage fade and voltage hysteresis. The activated material can be explained as a percolating network of higher-voltage, layered-type sites having facile Li diffusion. Interspersed throughout this network are lower-voltage, disordered sites that represent a significant barrier.

25 ENERGY STORAGE↗
DOE OSTI2022

Electrochemical Modeling and Experimental Verification of Lithiation Gradients in Oxide Cathodes of Lithium-Ion Cells

Lithiated nickel-cobalt-manganese oxides, such as NCM523, are used in the positive electrode (cathode) of Li-ion cells. Using operando X-ray diffraction profilometry, lithiation gradients in the cathode matrix can be observed and quantified by expansion into Legendre polynomials with time-dependent weights. These weights (referred to as gradients) increase in magnitude when electric current flows through the cell, decrease during potentiostatic hold and finally relax to zero when the current is interrupted during open circuit rest. Both physics-based electrochemical models and operando X-ray experiments suggest that the time constants for gradient growth and abatement are primarily determined by ionic diffusion in the oxide particles, which in turn depends on their lithium content. In contrast, the magnitude of gradients depends mainly on the applied current. The X-ray profilometry provides a way of directly probing the formation and disappearance of Li gradients across the cathode during fast cycling, which can help to diagnose the effects of material degradation in the cells.

25 ENERGY STORAGE↗
DOE OSTI2023

Evaluation of Cathode Materials with Lithium-Metal Anodes: Baseline Performance and Protocol Standardization of Coin Cells

The collaborative evaluation of electrode materials across multiple research entities requires standardized electrochemical testing protocols to produce reliable, one-to-one comparisons between different systems of interest. Similar to the work done by Long et al. on protocol standardization for coin-cell testing with graphite anodes [J. Electrochem. Soc., 163, A2999, (2016)], here we introduce two standardized testing protocols designed to quickly evaluate important electrochemical properties of cathode materials using lithium-metal anodes. The two protocols measure kinetic and thermodynamic capacity losses, rate- and voltage-dependent cycling capacities, instabilities at high voltage and high cycling rate, and overpotentials at various states of charge. We then apply these protocols to four commercially available cathode materials to establish benchmark performance metrics that can be used to screen and evaluate new cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2025

Mitigating Transition Metal Dissolution from Mn-rich Cathodes: Influence of Processing and Testing Methods

Manganese-rich oxides continue to gain interest with respect to the development of Earth-abundant options for lithium-ion cathodes. Of the unique challenges that hinder the respective performance of various classes of such materials, manganese dissolution still stands as a common theme. The work herein explores Li 3 PO 4 as a robust surface protection layer on a prototypical, Co-free, manganese-rich cathode in the way of a lithium- and manganese-rich oxide. The study highlights the critical importance of synthesis and processing in realizing optimal performance of a given surface treatment by comparing sol-gel and atomic layer deposition methods. Furthermore, cycling protocols are emphasized as a critical factor in adequately gauging the efficacy of surface protection strategies to mitigate manganese dissolution and the subsequent electrochemical consequence. Optimized Li 3 PO 4 coatings coatings on lithium- and manganese-rich cathode particles are shown to greatly mitigate capacity fade, impedance rise, pore/void formation and mechanical damage during long-term cycling.

Mallick, Subhadip [Argonne National Laboratory (AN↗
DOE OSTI2025

Lithium-Ion Batteries with Lithium Manganese Iron Phosphate Cathodes and Lithium Titanate Anodes: Linking Electrode Dynamics to Cell Performance

This study examines the electrochemical performance, impedance behavior, and aging mechanisms of lithium-ion cells pairing lithium manganese iron phosphate (LiMn 0.6 Fe 0.4 PO 4 , LMFP64) cathodes with lithium titanate (Li 4 Ti 5 O 12 , LTO) anodes. LMFP64 half-cells display distinct Fe and Mn redox plateaus at ∼3.5 and ∼4.1 V, respectively, and deliver excellent rate capability. Three-electrode measurements show that LMFP64 dominates cell impedance, which changes sharply across the Fe–Mn redox transition and decreases with increasing temperature (30 °C–50 °C). Voltage hysteresis arises mainly from the cathode, with higher C-rates shortening redox plateaus and broadening the transition region. Elevated temperature lowers impedance, especially near the Mn-redox and transition regions, but accelerates capacity fade. Post-cycling analyses of electrodes confirm structural stability of LMFP64 and indicate loss of lithium inventory (LLI) as the source of capacity fade. This LLI causes potential slippage between the LMFP64 and LTO electrodes, which decreases the Fe-redox plateau width. Long-term cycling highlights the critical role of electrode overhang: cathode overhang mitigates capacity fade by buffering lithium loss, whereas anode overhang cells experience faster capacity decline due to uncompensated lithium depletion. These results clarify LMFP64/LTO battery impedance evolution, thermal effects, and degradation pathways and provide insights for their applications in electric vehicles.

Area Specific Impedance↗
DOE OSTI2016

A Spinel-integrated P2-type Layered Composite: High-rate Cathode for Sodium-ion Batteries

Sodium-ion batteries (SIB) are being intensively investigated, owing to the natural abundance and low cost of Na resources. However, the SIBs still suffer from poor rate capability due to the large ionic radius of Na+ ion and the significant kinetic barrier to Na+-ion transport. Here, we present an Fd-3m spinel-integrated P2-type layered composite (P2 + Fd-3m) material as a high-rate cathode for SIBs. The P2 + Fd-3m composite material Na0.50Ni1/6Co1/6Mn2/3O2 shows significantly enhanced discharge capacity, energy density, and rate capability as compared to the pure P2-type counterpart. The composite delivers a high capacity of 85 mA h g-1 when discharging at a very high current density of 1500 mA g-1 (10C rate) between 2.0 and 4.5 V, validating it as a promising cathode candidate for high-power SIBs. The superior performance is ascribed to the improved kinetics in the presence of the integrated-spinel phase, which facilitates fast electron transport to coordinate with the timely Na+-ion insertion/extraction. The findings of this work also shed light on the importance of developing lattice doping, surface coating, and electrolyte additives to further improve the structural and interfacial stability of P2-type cathode materials and fully realize their practical applications in sodium-ion batteries.

Zheng, Jianming↗
DOE OSTI2019

Water-Processable P2-Na 0.67 Ni 0.22 Cu 0.11 Mn 0.56 Ti 0.11 O 2 Cathode Material for Sodium Ion Batteries

Sodium ion batteries offer a low-cost, sustainable, and environment-friendly solution to large-scale electrochemical energy storage systems. Layered oxides represent a family of promising cathode materials with a potential to improve the energy and power densities while reducing the material cost of sodium ion batteries. However, due to the chemical and structural instability of layered oxides in an aqueous solution, the current battery electrode manufacturing requires expensive and hazardous organic solvents, which impedes the full benefit of the low-cost, sustainable, and eco-friendly advantages. We need an effective technology that empowers a cathode with water processable properties. In this study, we set a representative example, P2-Na0.67Ni0.22Cu0.11Mn0.56Ti0.11O2, to explore its performance under water-processing conditions. This material achieves a discharge capacity of 180 mAh/g and a discharge energy of 544 Wh/kg at 22 ?C. The aging experiments indicate its superior stability against water, having negligible bulk 2 structural or chemical changes. The surface sensitive soft X-ray absorption spectroscopy shows that the P2-Na0.67Ni0.22Cu0.11Mn0.56Ti0.11O2 has stable surface chemistry in the aqueous solution. Moreover, the cells with water-processed cathodes delivered stable cycling performance with minor voltage decay, originating from the decreased cell impedance. Therefore, the present study sets a refined example to establish a low-cost, sustainable, and eco-friendly solution by developing water-processable electrode materials for sodium ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2017

Mixed Polyanion Glass Cathodes: Mixed Alkali Effect

In lithium-ion batteries, mixed polyanion glass cathodes have demonstrated high capacities (200-500 mAh/g) by undergoing conversion and intercalation reactions. Mixed polyanion glasses typically have the same fundamental issues as other conversion cathodes, i.e.: large hysteresis, capacity fade, and 1st-cycle irreversible loss. A key advantage of glass cathodes is the ability to tailor their composition to optimize the desired physical properties and electrochemical performance. The strong dependence of glass physical properties (e.g., ionic diffusivity, electrical conductivity, and chemical durability) on the composition of alkali mixtures in a glass is well known and has been named the mixed alkali effect. The mixed alkali effect on battery electrochemical properties is reported here for the first time. Depending on glass composition, the mixed alkali effect is shown to improve capacity retention during cycling (from 39% to 50% after 50 cycle test), to reduce the 1st-cycle irreversible loss (from 41% to 22%), and improve the high power (500 mA/g) capacity (from 50% to 67% of slow discharge capacity).

Kercher, A. K.↗
DOE OSTI2022

Python catemis package for DARHT Axis-II Dispenser-Cathode Emissivity and Temperature Analysis

The catemis python package includes the analysis methods used in paper "DARHT Axis-II Dispenser-Cathode Emissivity and Temperature", which was presented at the 2021 Weapons Engineering Symposium and Journal (WESJ) hosted by Los Alamos National Laboratory. The paper (LA-UR-21-25647) and presentation (LA-UR-21-28231) report on a temperature and emissivity model that has been developed and applied to data from diagnostics used to measure the surface temperature of the DARHT Axis-II hot dispenser cathode over more than a decade of operation. The catemis package provides all the methods used in reporting these results along with the data files used to create the plots and tables in the paper. This includes methods for loading and processing FAR spectral pyrometer data along with methods for temperature calibration of cathode images.

Koglin, Jason↗