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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Tetrahedral Zn 2+ doping LiNi 0.6 Mn 0.2 Co 0.2 O 2 improves discharge capacity retention by altering surface Ni valence during cycling and preventing oxygen evolution

5 mol-% Zn 2+ was added to the co-precipitation synthesis of LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) to understand Zn's effect on the structural and electronic properties of NMC622. Zn is determined to successfully dope into the NMC crystal lattice as there is an increase in d-spacing along the [003], [104], and [110] directions and an increase in molar volume (100.75 cm 3 mol -1 for NMC622 and 101.00 cm 3 mol -1 for Zn-NMC). Through XPS, Zn is determined to dope on the tetrahedral 6c Wyckoff site in the NMC structure and TEM-EDS reveals that despite a slight ZnO impurity phase, 1.4 mol-% Zn successfully dopes into the crystal structure. Furthermore, cyclic voltammetry shows a suppressed anodic wave associated with oxygen evolution and EIS demonstrates that Zn-doped NMC decreases charge transfer resistance and increases Li diffusion by an order of magnitude. After the formation cycles, NMC has a higher 1 C accessible capacity, 141 mAh/g, over Zn-NMC (132 mAh/g), but after long term cycling Zn-NMC has a higher accessible capacity (117 mAh/g compared to 96 mAh/g for NMC) and increases discharge capacity retention by 18% leading to longer cycle life.

Electrochemistry↗
DOE OSTI2026

Structure–Property Relationships of Recycled Lithium-Ion Battery Cathodes: Microstructure Optimization Using Virtual Materials Testing

The increasing demand for sustainable battery technologies requires effective recycling strategies for end-of-life lithium-ion battery cathodes. In this study, virtual materials testing, a well-established framework for modeling conventionally manufactured NMC-based cathodes, is applied to partially recycled cathodes. To this end, virtual cathodes consisting of mixtures of pristine and recycled NMC particles are utilized to systematically analyze structure–property relationships depending on mixing ratios and different spatial arrangement strategies. For this purpose, a stochastic 3D model is developed that is capable of generating virtual cathodes with arbitrary volume fractions of active materials and mixing ratios of pristine and recycled NMC particles. Particularly, the stochastic 3D model can mimic the different size distributions of pristine and recycled particles that are observed in image data. Additionally, the model allows the structuring of pristine and recycled NMC either uniformly mixed or layer-wise arranged, mimicking single- and dual-layer cathodes. Subsequently, a systematic computational analysis is conducted to assess the influence of increasing active material ratios of recycled particles, ranging from 0 % to 100 %, while maintaining a constant overall active material volume fraction. The impact of particle mixing on cathode performance is evaluated by examining transport-relevant geometrical descriptors and effective properties, such as geodesic tortuosity, specific surface area, and tortuosity factor.

25 ENERGY STORAGE↗
DOE OSTI2024

Accurately constituting robust interfaces for high-performance high-energy lithium metal batteries

High-energy lithium metal batteries (LMBs) have received ever-increasing interest. Among them, coupling lithium metal (Li) with nickel-rich material, LiNi x Mn y Co z O 2 (NMCs, x ≥ 0.6, x + y + z = 1), is promising because Li anodes enable an extremely high capacity (∼3860 mA h g −1 ) and the lowest redox potential (−3.04 V vs. standard hydrogen electrode), while NMCs can achieve a much higher capacity of ∼200 mA h g −1 and lower cost than those of LiCoO 2 . However, the resultant Li‖NMC cells have been hindered from commercialization due to a series of challenges related to the interface stability of both Li anodes and NMC cathodes. Specifically, Li anodes suffer from Li dendritic growth and the formation of solid electrolyte interphase (SEI), while NMC cathodes suffer from the formation of cathode electrolyte interphase (CEI) and other interface-related issues, including transition metal dissolution, oxygen release, cracking, and so on. To tackle these issues, recently, two sister techniques, atomic and molecular layer deposition (ALD and MLD), have emerged and exhibit tremendous capabilities to accurately constitute robust interfaces to achieve high-performance Li‖NMC LMBs. They can uniquely develop uniform and conformal films as surface coatings of LMBs in a precisely controllable mode at the atomic/molecular level, while proceeding with film deposition at low temperatures (e.g., ≤250 °C). In this Feature Article, we review the latest research progress in developing novel surface coatings via ALD and MLD for Li‖NMC LMBs and discuss outcomes for pursuing high performance.

25 ENERGY STORAGE↗
DOE OSTI2024

North America’s Potential for an Environmentally Sustainable Nickel, Manganese, and Cobalt Battery Value Chain

The Detroit Big Three General Motors (GMs), Ford, and Stellantis predict that electric vehicle (EV) sales will comprise 40–50% of the annual vehicle sales by 2030. Among the key components of LIBs, the LiNixMnyCo1−x−yO2 cathode, which comprises nickel, manganese, and cobalt (NMC) in various stoichiometric ratios, is widely used in EV batteries. This review reveals NMC cathodes from laboratory research. Furthermore, this study examines the environmental effect of NMC cathode production for EV batteries (including coating technologies), encompassing aspects such as energy consumption, water usage, and air emissions. Although gaps persist in NMC cathode environmental assessments (NMC111, NMC532, NMC622, and NMC811), limited life cycle assessments “(LCA)” have been conducted. Most available data originate from Asia (primarily China), accounting for 85% of the production of EV LIB cathode materials. The concept of battery passports for data collection on LIB components has been proposed to facilitate material traceability as a system for ensuring a sustainable supply chain for critical minerals. The automotive industry’s shift to electrification necessitates a sustainable supply chain from mine to vehicle end-of-life. As the critical mineral supply moves from Asia to North America, environmentally friendly industrial methods must be studied to provide this supply chain direction.

25 ENERGY STORAGE↗
DOE OSTI2026

Thermal Stability of LiNi x Mn y Co z O 2 Cathode Materials

Here, the thermal evolution of LiNi x Mn y Co z O 2 (NMC) lithium-ion battery electrode materials is examined at various states of charge (SOC) or lithium concentrations for a variety of Ni:Mn:Co ratios or electrode compositions. Synchrotron X-ray diffraction (XRD) combined with Rietveld analysis shows the onset decomposition temperatures of phases, decomposition products, lattice parameters, and phase fractions as a function of composition and SOC. SOC impacts the lattice parameters of the NMC phase, where a collapse of the c-axis in the NMC phases is noted due to lithium extraction. Among the compositions examined, the low-Ni NMC111 uncycled sample (NMC111 0% SOC) exhibited the highest thermal stability, with a decomposition temperature approximately 250 °C higher than that of NMC532 0% and NMC811 0%. When the SOC exceeds 50% (i.e., more than 0.4 mol of Li ions extracted), the influence of Ni content on the decomposition temperature becomes negligible, with decomposition occurring around 250−300 °C for all compositions. Ni content also affects the decomposition pathways: NMC111 tends to first form a TM 3 O 4 -type phase, where TM represents transition metals, before transforming into a TMO-type phase, whereas most of the NMC811 samples directly decompose into the TMO phase. The presence of metallic phases was confirmed by both XRD and thermogravimetric-differential scanning calorimetry (TGA-DSC) analysis, as a result of heating under inert conditions. The TGA-DSC results suggest that metallic phase formation is favored at lower SOC in samples with a higher Ni content. This work provides comprehensive insight into the thermal degradation pathways of NMC materials as a function of composition, SOC, and temperature.

Peng, Jian [Univ. of New South Wales, Sydney, NSW ↗
DOE OSTI2025

Hydrogen density mapping in biomolecular crystals through dynamic nuclear polarization

Many fundamental biological processes, including those in photosynthetic reaction centers and enzyme active sites, involve charge and energy transfer, bond cleavage, protonation and hydrogen bonding. Because H atoms play such central roles in these reactions, accurately determining their positions is essential. Yet, conventional X-ray crystallography primarily resolves the heavy atoms in biological structures and provides limited insight into hydrogen, even at atomic resolution. Neutron macromolecular crystallography (NMC) overcomes this limitation by offering exceptional sensitivity to hydrogen and deuterium. Here, we present a theoretical framework for the development of dynamic nuclear polarization NMC (DNP-NMC) techniques, which exploit the alignment of neutron and proton nuclear spins to enhance and tune the hydrogen signal contribution. The DNP-NMC approach advances the resolution of H atoms within biomolecular crystals, whether bound to protein residues or present in solvent. The method establishes key relationships for the coherent structure factor of polarized neutron scattering from hydrogenous matter. It theoretically achieves full accuracy in phase reconstruction and offers a path to improve neutron structure determination, achieving accuracies exceeding ≳80% by incorporating titration states. Using a variant of the hybrid input/output phase-retrieval algorithm, it allows recovery of the hydrogen density with ≳90% phase accuracy. In conclusion, we further discuss sources of experimental uncertainty for the upcoming DNP-enabled, quasi-Laue IMAGINE-X experiment at Oak Ridge National Laboratory's High Flux Isotope Reactor.

dynamic nuclear polarization↗
DOE OSTI2026

Cost Competitive Process of Battery Grade Oxides Preparation from Aged LIBs

The increasing demand for lithium-ion batteries (LIBs) is driving development of advanced recycling and refining methods. In this project, new cathode active materials are prepared from recycled lithium battery materials and subsequently electrochemically evaluated in coin cells. In detail, scrap LIBs were mechanically processed into a metal rich black mass, then reductive acid leached into an aqueous metal solution, and finally high-purity metal hydroxide precursor materials were prepared by selective electrochemical flow precipitation. Closed-loop LIB recycling into active electrode materials will enable US manufacturers to break their reliance on foreign sources of critical materials. For example, electroextraction process used here has potential to significantly reduce chemical & water use as well as waste production as compared to traditional metallurgic techniques. To this end, electroextracted materials refined from used batteries were collected and processed to be tested as precursor cathode active material (pCAM). For this project, two samples of high purity recycled NMC hydroxide (~1 kg each) were received from N th Cycle’s Ohio demonstration facility. The NMC compositions of the two materials are similar, and the levels of impurities have been confirmed. Indeed, impurities like copper, boron and sodium are present in quantities that could negatively impact battery performance. However, some studies have demonstrated that the control of the quantity of elements like copper or boron may improve the electrochemistry properties of Lithium-NMC batteries. The principal objective is to determine the electrochemical performance of these 2 NMC hydroxide batches and clearly determine the effect of the impurities on the performance.

25 ENERGY STORAGE↗
DOE OSTI2025

Probing the Effect of Electrode Thermodynamics on Reaction Heterogeneity in Thick Battery Electrodes

Thick electrodes present a viable strategy for enhancing energy density and reducing manufacturing costs of lithium-ion batteries. However, reaction heterogeneity during cycling compromises their rate capability and cycle life. While this nonuniformity is commonly attributed to sluggish charge transport, it is demonstrated here that the thermodynamic properties of the electrode material play an equally critical role. Through combined X-ray fluorescence microscopy and absorption near-edge structure spectroscopy, reaction distributions in LiFePO 4 (LFP) and LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC) thick electrodes with matched porosity and tortuosity are compared. LFP electrodes develop pronounced depth-oriented state-of-charge (SOC) gradients that worsen with increasing discharge rates, whereas NMC maintains much more uniform SOC distributions under such conditions. This difference originates from their distinct SOC dependence of equilibrium potentials and is quantifiable through a dimensionless “reaction uniformity” number. Intriguingly, LFP thick electrodes also exhibit lateral SOC variations that strengthen during slow discharge. In conclusion, the enhanced reaction uniformity in NMC correlates with better active material utilization and slower capacity fade than LFP, highlighting electrode thermodynamics as a key design consideration for thick electrodes.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Selectively extracting lithium from single and mixed cathode materials

With the burgeoning reliance on lithium-ion batteries for sustainable energy solutions and electric transportation, the environmental and resource management associated with battery disposal are increasingly critical. Addressing these challenges necessitates innovative recycling techniques that recover valuable battery components, particularly lithium. This research introduces a universal, eco-friendly approach tailored for the efficient selective extraction of lithium from both single and mixed cathode materials, achieving impressive selective leaching efficiencies of lithium (99.51 % for LFP, 90 % for NMC, and 97.24 % for mixed cathode). Surprisingly, leaching efficiency of lithium from NMC can be significantly improved by introducing LFP since LFP can remove the dense transition-metal salts on the surface of NMC. The extracted lithium is recovered as lithium carbonate with battery-grade purity. This study also highlights the reuse of formic acid and the adoption of oxygen as an oxidizing agent to prevent wastewater production. Therefore, this method provides a robust foundation for sustainable lithium battery recycling.

economically and environmentally feasible↗
DOE OSTI2025

Characterizing Hazardous Gases from NMC811 Materials and Coin Cells with TGA and Tube-Furnace FTIR-MS Evolved-Gas-Analysis

Abuse testing is useful for informing the risks of different battery chemistries but has been limited to larger formats. This paper conducted thermal abuse tests at the smaller coin cell level to determine its relevance in specifying vent gas flammability and toxicity. A nitrogen purge carried the evolved gases into a parallel Fourier-transform infrared spectrometer (FTIR) and a mass spectrometer (MS) downstream of the tube furnace. The experimental system was validated by comparing evolved gas data for single components between the tube furnace system and a thermogravimetric analysis (TGA) instrument. Multiple samples were tested during validation, including CaCO3, electrolyte, delithiated NMC 811 cathode, and lithiated graphite anode. Temperature-resolved gas evolution of HF, CO2, CO, H2, and hydrocarbons from isolated components helped to characterize the emission sources. A previously unreported H2 generation mechanism was found. It was shown that the reduced NMC cathode acts as a catalyst to crack polypropylene-decomposed hydrocarbons into H2 at around 450 degrees C. It was also shown, while studying LiPF6 thermal decomposition, that using the tube furnace with a coin cell casing as the sample holder has some advantages for evolved-gas analysis of environmentally sensitive samples relative to testing in TGA instruments. After validation with single components, a fully charged NMC 811 coin cell was failed in the tube furnace. The measured evolved gases were found to be a combination of the species measured from the single component tests. H2 formation related to the reduced cathode was found to have greater abundance than H2 formed from the anode. Hydrogen fluoride emission factors and diethyl carbonate conversion emission factors assist in understanding the gaseous hazards for larger format cells.

25 ENERGY STORAGE↗
DOE OSTI2026

Daily operational impacts on battery degradation in heavy-duty electric drayage trucks

Battery aging is a critical factor influencing the performance, longevity, and cost of ownership of battery electric trucks (BETs). This paper presents a comprehensive evaluation of battery aging for two Li-ion battery chemistries, Nickel-Manganese-Cobalt (NMC) and Lithium-Iron-Phosphate (LFP), accounting for both cycling and calendar aging. In contrast to traditional methods that rely on simplified linear degradation models based on manufacturer-provided data, this study employs semi-empirical aging models calibrated to experimentally collected data. The models are integrated into a detailed vehicle simulation environment, enabling a comprehensive assessment of battery degradation under realistic operating conditions. A case study focusing on heavy-duty electric drayage truck operations in the Port of Savannah, GA, is presented to illustrate the impact on battery pack lifespan of: seasonal variations, daily operational activities, charging strategies, and battery storage conditions. The results illuminate the significance of the battery pack’s state of charge during stationary periods, such as overnight storage or weekend parking, on battery degradation and its potential implications for long-term vehicle viability. Additionally, the study explores how different operational and environmental factors affect battery degradation, offering critical insights into best battery charging and storage practices. Our results demonstrate that LFP outperforms NMC in terms of years of useful life; however, by utilizing charging strategies that minimize the amount of time the battery spends resting at high levels of state-of-charge, the lifespan of the battery pack that uses NMC can nonetheless be increased by more than a factor of two.

25 ENERGY STORAGE↗
DOE OSTI2026

Interfacial Chemistry Involved in Selective Separation of NMC/LMO and LCO/LMO Binary Cathode Materials by Froth Flotation Using Oleic Acid

The variability in cathode compositions within recycled lithium-ion battery (LIB) feedstocks poses a significant challenge to efficient downstream refining processes. This study demonstrates the feasibility of using froth flotation with oleic acid as a collector to selectively separate lithium nickel-manganese-cobalt oxide (NMC) and lithium cobalt oxide (LCO) from lithium manganese oxide (LMO) materials. Laboratory-scale flotation tests achieved an 80% separation efficiency in a single stage, producing a froth product with >90% purity of NMC/LCO at approximately 90% yield. Concurrently, the LMO materials were enriched in the sink product with ∼90% purity and ∼90% yield. This approach was further validated using recycled cathode materials, confirming its applicability to realistic feedstocks. The underlying mechanism governing the selective separation of NMC/LCO from LMO was investigated using ζ-potential measurements, contact angle measurements, bubble-particle attachment experiments, and X-ray photoelectron spectroscopy (XPS) analysis. Both contact angle and bubble-particle attachment results confirmed that oleic acid adsorption rendered NMC and LCO surfaces hydrophobic, thereby enhancing flotation recovery. At pH 5, oleic acid adsorbed preferentially onto NMC and LCO surfaces via electrostatic interactions, while exhibiting minimal adsorption on LMO surfaces. However, separation efficiency deteriorated at higher pH, which was attributed to the co-flotation of LMO materials caused by oleate chemisorption on MnOH + species. This work establishes froth flotation as a viable cathode/cathode separation strategy, providing a low-cost, scalable pathway to preconcentrate and enrich nickel-rich and cobalt-rich cathode active materials from incompatible cathode chemistries for direct recycling or hydrometallurgical processing. Furthermore, this study reveals, for the first time, the mechanism of oleate adsorption on the surface of different cathode materials.

PH↗
DOE OSTI2025

Ni-Rich Li[Ni x MnyCo 1– x – y ]O 2 Single Crystals as Superior Fast Charge Cathodes for Lithium-Ion Batteries

The utilization of single-crystal (SC) Li[Ni x MnyCo 1-x-y ]O 2 (NMC) cathodes has facilitated unparalleled performance in commercial high-energy lithium-ion batteries (LIBs). In the current study, we evaluate the application of SC cathodes in fast charge (FC)-LIBs where particle cracking is a predominant failure mechanism. Ni-rich SC-NMC samples with various compositions, sizes, and shapes are synthesized and investigated for their influence on FC performance. We reveal the necessity of utilizing smaller SCs (<1 μm) as larger sizes (>2 μm) experience significant particle-level lithium concentration gradients under FC conditions. To improve lithium transport and minimize side reactivities, we strategically expose the (104) crystal facets on the surface. Exceptional performance was observed on an optimized SC-LiNi 0.80 Mn 0.05 Co 0.15 O 2 , delivering a discharge capacity of 165 mAh/g even after 150 cycles at 6C charge. Our study not only demonstrates the promise of SC-NMC but also provides the key insights for the design and optimization of advanced cathodes for FC-LIBs.

25 ENERGY STORAGE↗
DOE OSTI2024

Decoupling first-cycle capacity loss mechanisms in sulfide solid-state batteries

Solid-state batteries (SSBs) promise more energy-dense storage than liquid electrolyte lithium-ion batteries (LIBs). However, first-cycle capacity loss is higher in SSBs than in LIBs due to interfacial reactions. The chemical evolution of key interfaces in SSBs has been extensively characterized. Electrochemically, however, we lack a versatile strategy for quantifying the reversibility of solid electrolyte (SE) redox for established and next-generation SSB electrolytes. In this work, we perform tailored electrochemical tests and operando X-ray diffraction to disentangle reversible and irreversible sources of capacity loss in positive electrodes composed of Li 6 PS 5 Cl SE, Li(Ni 0.5 Mn 0.3 Co 0.2 )O 2 (NMC), and carbon conductive additives. We leverage an atypically low voltage cutoff (2.0 V vs. Li/Li + ) to quantify the reversibility of SE redox. Using slow (5.5 mA g NMC −1 ) cycling paired with >100 h low-voltage holds, our cells achieve a surprising 96.2% first-cycle coulombic efficiency, which is higher than previously reported (mean: 72%, maximum: 91.6% across surveyed literature). We clarify that sluggish NMC relithiation kinetics have been historically mistaken for permanently irreversible capacity loss. In conclusion, through systematic decoupling of loss mechanisms, we uncover the unexpected reversibility of SE redox and isolate the major contributors to capacity loss, outlining a strategy for accurate assessment of next-generation SE materials and interface modifications.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Pushing the Limits: Maximizing Energy Density in Silicon Sulfide Solid‐State Batteries

Here, for the first time, we demonstrate a silicon solid-state battery (SSB) architecture that achieves >400 Wh kg −1 , approaching the theoretical limit for silicon-based SSBs. This configuration features a 99.9 wt% micro-Si, a thin sulfide solid electrolyte (SSE), and a high-loading NMC811. Key to these results is strategically selecting and evaluating the processing techniques, whether wet or dry, for the negative electrode, positive electrode and thin sheet-type SSE. Excessive lithium incorporation into the silicon host, beyond the Li 3.75 +Si phase to form a LiSi composite, is essential to match the high capacity of the positive electrode. This SSB achieves over 1000 cycles for a 2 mAh cm −2 with ≈80% capacity retention and 94% capacity retention for 3 mAh cm −2 over 500 cycles at 25 °C. Post analysis identifies the primary capacity decay mechanisms as oxidation at the NMC/SSE interface and structural disruptions within NMC. Meanwhile, the Si electrode maintains a robust solid-electrolyte interphase layer, minimizing capacity decay. This study highlights the necessity for improved NMC coatings, lattice oxygen stabilization, and a durable positive electrode-electrolyte interface to improve the long-term stability of SSBs. Strategies leading to a single-layer pouch cell SSB exceeding 400 Wh kg −1 are developed.

25 ENERGY STORAGE↗
DOE OSTI2025

Heterogeneity of the Dominant Causes of Performance Loss in End-of-Life Cathodes and Their Consequences for Direct Recycling

Recycling Li-ion batteries from electric vehicles is critical for reducing costs and supporting the development of a domestic battery supply chain. Direct recycling of cathodes, like LiNixMnyCozO2 (NMC), is attractive due to its low cost, energy use, and emissions compared to traditional recycling techniques. However, a comprehensive understanding of the active material properties at end-of-life is needed to guide direct recycling processes and the performance-dependent reuse applications. Here, NMC material from an end-of-life commercial pouch cell is characterized and bench-marked against pristine non-cycled counterparts with respect to capacity, impedance, crystallography, morphology, and microstructure to identify major degradation modes and understand variability in the end-of-life material. The spatial heterogeneity of each property throughout the cell is also quantified. While the degraded material demonstrated similar capacity as the pristine, its impedance and rate capability are severely diminished. Furthermore, samples from the periphery of the electrode layers showed more severe performance loss compared to samples extracted from central regions. The dominant culprit of performance loss is the material microstructure, where the magnitude of particle cracking showed the strongest correlation to the impedance components that are most unfavorably impacted. This work suggests severe cracks in cathode active materials are the primary challenge that direct recycling methods must overcome.

25 ENERGY STORAGE↗
DOE OSTI2025

Flux Upcycling of Degraded Layered Cathodes to LiNi x Mn y Co z O 2 (NMCs) with Gradient Transition Metal Distribution

The rising demand for lithium-ion batteries (LIBs) has intensified the need for efficient recycling methods to address both supply chain constraints and environmental impacts. Direct upcycling, distinguished by its ability to achieve both the structural and compositional integrity of cathode materials, has gained prominence as a sustainable alternative to conventional pyrometallurgical and hydrometallurgical processes. However, the current direct upcycling methods are typically limited by incorporating Li and/or Ni, significantly constraining the adaptability across diverse LiNi x Mn y Co z O 2 (NMCs). Here, in this study, a versatile molten salt approach is reported that expands the scope of direct upcycling by enabling simultaneous incorporation of Li, Ni, and Mn. This methodology facilitates flexible conversion among diverse NMC compositions, including non-stoichiometric Co/Mn systems such as upcycling degraded LiCoO 2 (D-LCO), LiNi 1/3 Mn 1/3 Co 1/3 O 2 (D-NMC111), LiNi 0.8 Mn 0.1 Co 0.1 O 2 (D-NMC811) to surface Mn enriched NMC111, LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC532), and NMC811, respectively. The gradient transition metal distribution in upcycled products, characterized by Mn-enriched outer layers and Co/Ni-enriched cores enhances the interfacial stability of NMC cathodes, addressing critical challenges in long-term performance and structural integrity. These results highlight the potential of flux methods for advancing the upcycling of spent cathodes and producing high-performance materials for next-generation LIBs applications.

lithium -ion batteries↗
DOE OSTI2025

Addressing Inherent Challenges to Chemical Relithiation of Cycled End‐of‐Life Cathode Materials

Recycling end‐of‐life (EOL) lithium‐ion batteries (LIBs) is important to retain valuable resources from critical materials present in EOL battery waste. Direct recycling methods offer an opportunity to recover intact valuable cathode materials with minimal re‐processing. An important step of the direct recycling process is relithiation which is used to restore lithium content to EOL cathode materials. However, little has been done to study how preprocessing steps such as washing or binder removal may affect relithiation methods in the direct recycling process. Here, the evolution of fluorine byproducts left over from preprocessing steps during a low‐temperature chemical redox mediator relithiation process is tracked. A facile washing step is presented as a solution for mediating adverse effects of surface contamination on the chemical relithiation performance. The structure, lithium content, and electrochemical performance of relithiated EOL NMC 622 material that underwent a pre‐relithiation washing step to remove fluorine byproducts is shown to match that of pristine NMC 622. In this work, it is showed that redox mediator relithiation as a part of a direct recycling process is a promising low energy method that can be applied to EOL material with inherent surface impurities if the proper pre‐relithiation processing steps are implemented.

25 ENERGY STORAGE↗