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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Examples of X-Ray Characterization Techniques in Energy Storage Research

Lithium-ion batteries have revolutionized the portable electronics and transportation sectors. Their performance is often critically dependent on the crystal structures of the anode and cathode electrode materials, which must enable the transport and reversible storage of lithium ions into and out of the lattice. Because lithium is a low-Z element, characterization of materials for lithium-ion batteries can be particularly challenging. Regardless, X-ray techniques enable analysis of material structures to better understand how battery materials perform and degrade, particularly when combined with other materials characterization and electrochemical characterization techniques. While X-ray techniques are most often used in battery research for phase identification of crystal structures, X-ray characterization techniques are also used for a wide variety of other purposes. I will discuss several examples from my research with various collaborators on several projects that highlight the impact that X-ray characterization techniques can have on battery research. The first example will focus on low-temperature microwave-assisted solvothermal synthesis of vanadium-doped LiFePO4 cathode materials for lithium-ion batteries. (1,2) Through a combination of electrochemical and materials characterization, we determined that low temperature synthesis resulted in metastable phases that enabled incorporation of higher dopant levels than resulting from high-temperature synthesis of thermodynamically stable phases. Rietveld refinement of X-ray diffraction data enabled understanding of how lattice parameters changed with doping levels and synthesis temperature. X-ray absorption near edge spectroscopy enabled understanding of the vanadium and iron oxidation states to confirm how vacancies in the structure caused by doping were charge compensated. This was important to understand because the literature suggests doping can improve LiFePO4 electrical conductivity, which improves battery charge and discharge rates. The second example will focus on understanding residual strain in lithium metal anodes. Lithium-ion batteries typically use graphite anodes, but the charge-storage capacity can be theoretically improved ~10x by using lithium metal as the anode material instead. However, lithium anodes suffer from growth of high-aspect-ratio features, such as dendrites, that can pierce nanoporous polymer separators and lead to short circuits and fires. External pressure is commonly applied to cells to enable better morphological control. We hypothesized that applied pressure may promote strain and possibly work hardening during electrochemical cycling, which motivated us to look for evidence of residual strain in lithium metal cycled under applied pressure using X-ray diffraction and sin2(..psi..) analysis. We found that lithium electrodeposited under high pressure exhibited in-plane compressive strain and that that lithium electrodeposited under low pressure did not. (3) The residual strain that accompanies electrodeposition under high pressure may lead to work hardening, which may explain how a soft metal like lithium can puncture separators and why higher pressure does not always decrease short circuits. (4-6) References: 1) Harrison, K. L.; Manthiram, A. Microwave-Assisted Solvothermal Synthesis and Characterization of Metastable LiFe1- x (VO) x PO4 Cathodes. Inorganic chemistry 2011, 50(8), 3613-3620. 2) Harrison, K. L.; Bridges, C. A.; Paranthaman, M. P.; Segre, C. U.; Katsoudas, J.; Maroni, V. A.; Idrobo, J. C.; Goodenough, J. B.; Manthiram, A. Temperature Dependence of Aliovalent-Vanadium Doping in LiFePO4 Cathodes. Chemistry of Materials 2013, 25(5), 768-781. 3) Rodriguez, M. A.; Harrison, K. L.; Goriparti, S.; Griego, J. J.; Boyce, B. L.; Perdue, B. R. Use of a Be-Dome Holder for Texture and Strain Characterization of Li Metal Thin Films via Sin2 (..psi..) Methodology. Powder Diffraction 2020, 35(2), 89-97. 4) Jungjohann, K. L.; Gannon, R. N.; Goriparti, S.; Randolph, S. J.; Merrill, L. C.; Johnson, D. C.; Zavadil, K. R.; Harris, S. J.; Harrison, K. L. Cryogenic Laser Ablation Reveals Short-Circuit Mechanism in Lithium Metal Batteries. ACS Energy Letters 2021, 6(6), 2138-2144. 5) Harrison, K. L.; Merrill, L. C.; Long, D. M.; Randolph, S. J.; Goriparti, S.; Christian, J.; Warren, B.; Roberts, S. A.; Harris, S. J.; Perry, D. L. Cryogenic Electron Microscopy Reveals That Applied Pressure Promotes Short Circuits in Li Batteries. Iscience 2021, 24(12). 6) Harrison, K. L.; Goriparti, S.; Merrill, L. C.; Long, D. M.; Warren, B.; Roberts, S. A.; Perdue, B. R.; Casias, Z.; Cuillier, P.; Boyce, B. L. Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME. ACS Applied Materials & Interfaces 2021, 13(27), 31668-31679.

batteries↗
DOE OSTI2024

3D Printed Nanoporous Separators Based on Polymerization-Induced Phase Separation for Fast-Charging, High Cycling Stability Li-Ion Batteries

Fast charging and stable lithium-ion batteries (LIBs) require prompt Li ion transport between electrodes. 3D porous separators can potentially improve ion transport at both the microscale and macroscale levels. Additive manufacturing (AM) is an ideal tool to produce and study 3D porous separators of LIBs, although little work has been reported in this area. Here, we demonstrate porous structural control in layer-by-layer printed hexanediol diacrylate (HDDA) separators using a projection micro stereolithography (PμSL) AM technology and present their corresponding battery performance in lithium nickel manganese cobalt oxide (NMC)/graphite full cells. The composition of photocurable resin determines the porous morphology (e.g., bicontinuous and droplet-like), while the settings of printing layer thickness and number of exposures can be used to adjust the porosity (e.g., from 27% to 63%). Optimal resin and print conditions are determined, and the resulting separator exhibits superior Li ion conductivity and therefore higher rate performance and longer cycling life. Compared with a Celgard 2325 separator, the optimized porous HDDA separator increases the 10C-rate capacity by 34% and decreases the capacity degradation rate at the 1C-rate by 4.9%. In conclusion, this work paves the way for future AM of 3D separators for high-energy, high-power, and long-cycling-life LIBs.

25 ENERGY STORAGE↗
DOE OSTI2022

Resolving Current-Dependent Regimes of Electroplating Mechanisms for Fast Charging Lithium Metal Anodes

Poor fast-charge capabilities limit the usage of rechargeable Li metal anodes. Understanding the connection between charging rate, electroplating mechanism, and Li morphology could enable fast-charging solutions. In this report we develop a combined electroanalytical and nanoscale characterization approach to resolve the current-dependent regimes of Li plating mechanisms and morphology. Measurement of Li + transport through the solid electrolyte interphase (SEI) shows that low currents induce plating at buried Li||SEI interfaces, but high currents initiate SEI-breakdown and plating at fresh Li||electrolyte interfaces. The latter pathway can induce uniform growth of {110}-faceted Li at extremely high currents, suggesting ion-transport limitations alone are insufficient to predict Li morphology. At battery relevant fast-charging rates, SEI-breakdown above a critical current density produces detrimental morphology and poor cyclability. Thus, prevention of both SEI-breakdown and slow ion-transport in the electrolyte is essential. This mechanistic insight can inform further electrolyte engineering and customization of fast-charging protocols for Li metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2025

Concavity-based local erosion and sphere-size-based local dilation applied to lithium-ion battery electrode microstructures for particle identification

Performance metrics of lithium-ion batteries can be extracted from the analysis of electrode microstructures nanoscale imaging. The characterization workflow can involve a challenging particle identification, or instance segmentation, step. In this work, we propose a new identification method based on an original transformation: a sphere-size-based local dilation followed by a concavity-based local erosion, that is local morphology closing. The new transformation is much more efficient than the global morphology closing, with correct identification achieved with only 1.7 % dilation volume and 2.6 % erosion volume on a test geometry, compared to 39.2 % and more than 50 %, respectively, with its global counterpart. The new method has been then benchmarked versus other identification algorithms (watershed and pseudo coulomb repulsive field) on a real electrode microstructure with equal or better segmentation achieved.

25 ENERGY STORAGE↗
DOE OSTI2022

Stability Enhancement and Microstructural Modification of Ni-Rich Cathodes via Halide Doping

In this study, elemental doping is an effective strategy to modify surface and bulk chemistry in NMC cathode materials. By adding small amounts of lithium halide salts during the calcination process, the Ni-rich NMC811 cathode is doped with Br, Cl, or F halogens. The dopant type has a significant impact on the lithiation process and heavily influences the final cathode porosity and surface morphology. Utilizing a variety of electrochemical, surface, and bulk characterization techniques, it is demonstrated that an initial content of 5 mol % LiBr or LiCl in the lithium source is effective in improving capacity retention while also providing excellent rate performance. The improvements are attributed to a substantial increase in specific surface area, the formation of a stable cathode electrolyte interface (CEI) layer, and suppressed surface reconstruction. In addition, the particle microstructure is better equipped to handle cyclic volume changes with increased values of critical crack lengths. Overall, it is demonstrated that anion doping via the addition of lithium halide salts is a facile approach toward Ni-rich NMC modification for enhanced cathode performance.

25 ENERGY STORAGE↗
DOE OSTI2026

Exfoliation of Cu-Containing Poly(triazine imide): From Three-Dimensional to Two-Dimensional Particle Morphology

Controlling the morphological parameters of extended covalent organic frameworks remains challenging and represents an important yet often elusive metric of consideration. Typically, carbon nitride materials possess local ordering but remain largely amorphous in terms of their long-range order and orientation. This study probes the synthesis of a crystalline carbon nitride, poly(triazine imide) lithium bromide which possesses an atomically-precise extended structure, and demonstrates its exfoliation into a two-dimensional hexagonal sheet-like morphology. Furthermore, a previously unreported carbon nitride material, poly(triazine imide) copper bromide, or PTI-CuBr, was developed through an additional flux-assisted cation-exchange process and is shown to retain its internal Cu cations during solvothermal exfoliation. Characterization by dynamic light scattering and high-angle annular dark-field scanning electron microscopy reveals the morphological changes and captures the high aspect ratio of the thin carbon nitride sheets with <10 nm thickness while maintaining hundreds of nm in width. Additional characterization by energy-dispersive spectroscopy and X-ray photoelectron spectroscopy confirms that the Cu:Br:N molar ratio was maintained within the extended layers throughout the exfoliation process. This top-down synthesis approach differs from typical methods that isolate thin sheets for subsequent metal−cation coordination and illustrates the importance of maintaining oxygen-free conditions to minimize copper clustering. Thus, this new approach is demonstrated to provide a consistent and more homogeneous occupancy of the PTI pore spaces throughout the carbon nitride framework.

Exfoliation↗
DOE OSTI2024

Heterogeneous Solid Electrolyte Interphase Interactions Dictate Interface Instability in Sodium Metal Electrodes

Sodium (Na) metal batteries have attracted recent attention due to their low cost and high abundance of Na. However, the advancement of Na metal batteries is impeded due to key challenges such as dendrite growth, solid electrolyte interphase (SEI) fracture, and low Coulombic efficiency. This study examines the coupled electro‐chemo‐mechanical interactions governing the electrodeposition stability and morphological evolution at the Na/electrolyte interface. The SEI heterogeneities influence transport and reaction kinetics leading to the formation of current and stress hotspots during Na plating. Further, it is demonstrated that the heterogeneity‐induced Na metal evolution and its influence on the stress distribution critically affect the mechanical overpotential, contributing to a faster SEI failure. The analysis reveals three distinct failure mechanisms—mechanical, transport, and kinetic—that govern the onset of instabilities at the interface. Finally, a comprehensive comparative study of SEI failure in Na and lithium (Li) metal anodes illustrates that the electrochemical and mechanical characteristics of the SEI are crucial in tailoring the anode morphology and interface stability. This work delineates mechanistic stability regimes cognizant of the SEI attributes and underlying failure modes and offers important guidelines for the design of artificial SEI layers for stable Na metal electrodes.

25 ENERGY STORAGE↗
DOE OSTI2021

On the crystallography and reversibility of lithium electrodeposits at ultrahigh capacity

Abstract Lithium metal is a promising anode for energy-dense batteries but is hindered by poor reversibility caused by continuous chemical and electrochemical degradation. Here we find that by increasing the Li plating capacity to high values ( e.g ., 10–50 mAh cm −2 ), Li deposits undergo a morphological transition to produce dense structures, composed of large grains with dominantly (110) Li crystallographic facets. The resultant Li metal electrodes manifest fast kinetics for lithium stripping/plating processes with higher exchange current density, but simultaneously exhibit elevated electrochemical stability towards the electrolyte. Detailed analysis of these findings reveal that parasitic electrochemical reactions are the major reason for poor Li reversibility, and that the degradation rate from parasitic electroreduction of electrolyte components is about an order of magnitude faster than from chemical reactions. The high-capacity Li electrodes provide a straightforward strategy for interrogating the solid electrolyte interphase (SEI) on Li —with unprecedented, high signal to noise. We find that an inorganic rich SEI is formed and is primarily concentrated around the edges of lithium particles. Our findings provide straightforward, but powerful approaches for enhancing the reversibility of Li and for fundamental studies of the interphases formed in liquid and solid-state electrolytes using readily accessible analytical tools.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Advancing the Performance of Lithium-Rich Oxides in Cooperation with Inherent Complexities: Engineering Domain Structure

The nanodomain structure of lithium- and manganese-rich, composite cathode materials has been systematically altered through synthesis conditions while keeping larger-scale morphological differences to a minimum. Clear changes in electrochemical performance across the samples studied are observed, especially with respect to the anomalous impedance at low states-of-charge. Atomic-scale modeling, coupled to electrochemical measurements and physical characterization, reveals the local consequences of the high-voltage activation charge process as a function of specific domain structures. Furthermore, the results explain the influence of different postactivation structures on the insertion of Li-ions and the associated impedance during discharge. This work adds to our series of studies on lithium- and manganese-rich oxides, demonstrating that the inherent performance of LMRs can be greatly enhanced through rational, highly controlled synthetic strategies based on an understanding of synthesis–structure–property relationships across length scales.

25 ENERGY STORAGE↗
DOE OSTI2022

Physicochemical Heterogeneity in Silicon Anodes from Cycled Lithium-Ion Cells

The severe capacity fade of lithium-ion cells with silicon-dominant anodes has hindered their widescale commercialization. In this work, we link cell capacity fade to the heterogeneous physicochemical evolution of silicon anodes during battery cycling. Through a multi-length scale characterization approach, we demonstrate that silicon particles near the anode surface react differently than those near the copper current collector. In particular, near the anode surface we find an amorphized wispy silicon encased in a highly fluorinated matrix of electrolyte-reduction products. In contrast, closer to the current collector, the silicon retains more of its initial morphology and structure, suggesting the presence of isolated particles. Here, the results show that accessibility of active silicon to lithium-ions varies across the anode matrix. Material and cell designs, which minimize electrode expansion resulting from the in-filling of pores with the solid electrolyte interphase (SEI), are needed to enhance anode homogeneity during the electrochemical cycling.

25 ENERGY STORAGE↗
DOE OSTI2022

Nanotomographic observation and statistical analysis of overcharging induced cracks in LiCoO 2 single crystalline particles

Particle fracture represents an important mode of battery electrode degradation. Extensive cracking occurs in the layered oxide cathodes of lithium-ion rechargeable batteries when they are charged beyond safe operational voltages. In this paper, we analyze the morphology and distribution of cracks in over 100 overcharged LiCoO 2 (LCO) single-crystalline particles imaged via X-ray nanotomography. Herein, we observe a strong particle size dependence in both nucleation and growth of cracks, with percentage of cracked particles, crack size, and crack surface area per unit volume all increasing significantly with particle volume. Increasing the cutoff voltage above 4.6V is found to trigger much more pronounced crack growth, which we attribute to the large misfit stress caused by the H1-3 to O1 phase transition. This study offers valuable statistical insights into the fracture behavior of layered oxide cathodes and reveals the importance of particle size control on electromechanical degradation of battery electrodes.

25 ENERGY STORAGE↗
DOE OSTI2025

Local Cation-Ordered Superlattice Stabilizing Ni-Rich Single-Crystalline Cathodes

Ni-rich single-crystalline cathodes are pivotal for advancing lithium-ion battery technology due to their high energy density and mechanical stability. However, Ni-rich single-crystalline particles face intrinsic structural heterogeneity due to excessively high sintering temperature required to shape micron-sized morphologies─typically over 150 °C above the polycrystalline optimum, leading to rapid electrochemical decay and unsatisfied rate performance that hinder their practical application. Here, in this work, we propose a lithium-deficient presintering strategy to synthesize cation-ordered single-crystalline LiNi 0.83 Co 0.12 Mn 0.05 O 2 (S-NCM83), effectively minimizing lattice chemical heterogeneity and defect formation. The resulting cation-ordered percolation network enhances the structural stability of the bulk, reduces the energy barrier for Li + migration, and stabilizes Li + diffusion pathways. Consequently, S-NCM83 demonstrates significantly improved cycling stability across various operating temperatures and achieves exceptional rate performance, delivering 206 mAh g –1 at 0.1 C and 170 mAh g –1 at 5 C, without requiring surface coatings or doping. This work introduces a universal strategy to address the long-standing structural instability issues in single-crystalline cathodes, paving the way for simplified and scalable approaches to long-life and high-energy lithium-ion batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Nondestructive flash cathode recycling

Effective recycling of end-of-life Li-ion batteries (LIBs) is essential due to continuous accumulation of battery waste and gradual depletion of battery metal resources. The present closed-loop solutions include destructive conversion to metal compounds, by destroying the entire three-dimensional morphology of the cathode through continuous thermal treatment or harsh wet extraction methods, and direct regeneration by lithium replenishment. Here, we report a solvent- and water-free flash Joule heating (FJH) method combined with magnetic separation to restore fresh cathodes from waste cathodes, followed by solid-state relithiation. The entire process is called flash recycling. This FJH method exhibits the merits of milliseconds of duration and high battery metal recovery yields of ~98%. After FJH, the cathodes reveal intact core structures with hierarchical features, implying the feasibility of their reconstituting into new cathodes. Relithiated cathodes are further used in LIBs, and show good electrochemical performance, comparable to new commercial counterparts. Life-cycle-analysis highlights that flash recycling has higher environmental and economic benefits over traditional destructive recycling processes.

25 ENERGY STORAGE↗
DOE OSTI2021

Orientation-Dependent Distortion of Lamellae in a Block Copolymer Electrolyte under DC Polarization

Lithium-salt-doped block copolymers have the potential to serve as solid electrolytes in rechargeable batteries with lithium metal anodes. In this work, we use small-angle X-ray scattering (SAXS) to study the structure of polystyrene-block-poly(ethylene oxide) (PS-b-PEO) doped with bis-(trifluoromethylsulfonyl)amine lithium salt (LiTFSI) during direct current (dc) polarization experiments in lithiu-lithium symmetric cells. The block copolymer studied is nearly symmetric in composition, has a total molecular weight of 39 kg mol -1 , and exhibits a lamellar morphology at all studied salt concentrations. When ionic current is passed through the electrolyte, a salt concentration gradient forms that induces a spatial gradient in the domain spacing, d. The dependence of d on distance from the positive electrode, x, was determined experimentally by scanning the incident X-ray beam from one lithium electrode to the other. By studying the two-dimensional (2D) SAXS patterns as a function of azimuthal scattering angle, we find that lamellae with PS/PEO interfaces oriented perpendicular to the flow of ionic current (LAM ⟂ ) swell and contract to a greater degree than those with interfaces oriented parallel to the current direction (LAM || ). While domains with the LAM ⟂ do not provide direct conducting pathways between the electrodes, our analysis suggests that they play an important role in establishing the salt concentration gradient necessary for sustaining a large ionic current through greater expansion and contraction.

25 ENERGY STORAGE↗
DOE OSTI2024

Unveiling Morphology and Crystallinity Dynamics in Ni x Mn 1– x CO 3 Cathode Precursors through Batch-Mode Coprecipitation

This study delves into the synthesis and control of Ni x Mn 1–x CO 3 , a critical class of Mn-rich, Co-free precursors vital for cathode-oxide materials in energy storage and conversion technologies. Employing batch-mode coprecipitation, we systematically generated samples with varying Ni concentrations (x = 0, 0.1, 0.3, 0.5, 0.7, and 0.9) and conducted a comprehensive analysis of their compositions, crystallinities, transition-metal distributions, and particle morphologies through both experimental and computational methods. A significant variation in particle size and crystallinity was observed, contingent on the Ni content. Further, a pivotal transition emerged at Ni concentrations above x = ~0.5, transforming uniform morphologies, such as spherical, monodisperse, pseudo-single-crystalline particles, into bimodal, polycrystalline structures. Furthermore, the study highlights the role of Ni–ammonia complexes leading to Ni-deficient precipitates and underscores the importance of ammonia concentration in achieving precise Ni content control. This study unveils critical reaction conditions governing Mn-rich precursor properties that are vital for cathode-oxides, emphasizing the need for meticulous synthetic control and offering the potential for practical applications in advanced energy storage and conversion systems.

25 ENERGY STORAGE↗
DOE OSTI2023

Understanding Biases in Sample Preparation Techniques for Coupled Scanning Electron Microscopy and MAMA PuO 2 Morphological Analysis

In this project, the scanning electron microscopy (SEM) sampling method used during the statistical design study (SDS) was investigated to determine if any sampling biases were present in the analyzed data. Using standard particle size distribution powders from the National Institute of Standards and Technology (NIST 1984 standard reference material) with the origin wet dispersion method, it was determined that a bias to smaller particles was present. This was supported by theoretical calculations using Stokes’ law to determine the settling rate of spherical particles of roughly the same size and mass as those found in the SDS. Based on the theoretical calculations, it was determined that the settling rate for each of the 76 powder sets in the SDS could be unique based on specific particle shape and mass distributions, making a universal correction factor/formula not applicable. Therefore, priority shifted to developing an improved wet dispersion method that significantly reduced the particle settling rate for all particle size and shapes. This was achieved by replacing the original solvent (isopropyl alcohol) with a heavy liquid (lithium heteropolytungstates), which dramatically slowed the settling rate and allowed for the capture of a suitable homogeneous aliquot. SEM imaging and Morphological Analysis for Material Attribution (MAMA) software analysis were conducted on the NIST standard, and the SEM/MAMA data were compared to data captured by a dynamic image analysis particle size analyzer. The resulting data confirmed that the new wet dispersion method does indeed deliver an improved representative aliquot to the SEM stub. For instance, in the NIST certificate, the average particle size is ~17.1 µm ± 2.2 µm with a normal distribution. The initial wet dispersion method resulted in a drastically reduced average particle size of 6.1 µm in addition to a non-representative heavy bi-modal distribution whereas the improved LST wet dispersion method resulting in an average particle size that was much closer to the NIST certificate (12.7 µm) with a similar normal distribution. Although the improved method was still short of the NIST certificate average, atomic force microscopy analysis determined that the resulting ~20-25% reduction in size was due to particles sinking into the carbon sticky tape used for SEM imaging. It is believed that that this bias can be calibrated in a much more predicable manner than the original settling rate bias. In addition, the matching normal distribution curves between the NIST certificate and the heavy liquid method indicate a much-improved representative aliquot has been sampled and imaged. A surrogate CeO 2 powder was used to reflect PuO 2 more accurately and to aid in implementing radiological controls and shielding. The resulting data sets from the SEM/MAMA method and the particle size analyzer give almost identical average particle sizes and particle distribution statistics. Future work will re-analyze several select runs from the SDS to determine if morphological signatures can be found with the improved sampling method.

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

Multiscale Modeling Framework for Lithium Nucleation in 3D Porous Carbon Anodes

Porous carbon scaffolds offer a promising route for mitigating non-uniform lithium (Li) plating to enhance the safety and longevity of Li metal batteries. However, the influence of microstructural morphology on Li nucleation is not well understood. Here, we present a multiscale modeling framework to investigate how the porous microstructure of carbon materials affects Li nucleation behavior. Ab initio molecular dynamics simulations quantify the nucleation energy barriers of Li on graphene as a function of Li content, surface curvature, and applied potential, providing key parameters for a classical nucleation theory (CNT) model. From macroscale half-cell simulations, we obtained Li concentration and electrical potential profiles to define boundary conditions for mesoscopic simulations. At the mesoscale, three distinct synthetic 3D microstructures with different porosities and characteristic feature sizes are generated to resolve local distributions of Li flux, current density, and mechanical stress. These outputs are integrated into the CNT model to map spatial variation in nucleation rates. Our findings reveal trade-offs between suppressing nucleation rates and achieving spatial uniformity, offering design guidelines for optimizing porous carbon anodes to balance nucleation control and mechanical integrity.

Materials science↗
DOE OSTI2024

Direct reuse of graphite and lithium nickel manganese cobalt oxide (NMC) recovered from ultrafast-laser ablation debris in Li-ion battery electrodes

Here we demonstrate that debris collected from the ultrafast-laser ablation of graphite anodes can be directly reused in a lithium-ion battery with little to no negative effects on electrochemical performance. Further, we show that while post-ablation NMC (LiNi 0.33 Mn 0.33 Co 0.33 O) cathode debris will require additional processing before being incorporated into an electrode, its critical materials (nickel, manganese, and cobalt) are not lost during ablation and can be recovered for recycling. Pre- and post-ablation materials are characterized with a suite of diagnostics, including SEM, TEM, X-ray CT, EDS, and XRD, to study changes in material morphology, composition and crystal structure. Graphite exhibited little to no morphological or compositional changes and a slight annealing of its crystal structure. NMC underwent profound morphological and crystallographic changes, but retained its elemental composition. Finally, post-ablation materials were re-manufactured into electrodes and cycled vs lithium metal. Graphite showed equal or better capacity and Coulombic efficiency compared to pre-ablation electrodes, while the post-ablation NMC exhibited severely reduced electrochemical performance. Furthermore, we discuss the outlook for application of this work to advanced manufacturing lines that produce next-generation, laser-patterned electrodes.

25 ENERGY STORAGE↗