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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Slug-flow synthesis of NCMA: Effect of substitution of cobalt with aluminum on the electrochemical performance of Ni-rich cathode for lithium-ion battery

Nickle-rich Li[Ni 1-x-y Co x Mn y ]O 2 (x, y≤0.1) (NCM) layered materials are known as promising cathode materials for next-generation lithium-ion batteries and electric vehicles owing to their high-reversible capacity and operating voltage of up to 3.6 vs Li/Li + . However, issues, such as irreversible phase transition, cation mixing, microcrack formation, thermal and structural stability of the material prevent its widespread adoption. Although, cation doping is a well-known technique to enhance the electrochemical performance of the NCM-based cathode material, the performance of the material is very sensitive to the doping amount. In this study, three Al-doped quaternary Ni-rich cathode materials Li[Ni 0.85 Co (0.1-x) Mn 0.05 Al x ]O 2 (where, x=0–0.04) (NCMA) are synthesized through three-phase slug-flow based continuous manufacturing process followed by high temperature calcination to study the effect of Aldoping on the performance of the cathode material while reducing Co. The slug flow-based production platform has several advantages, like particle size uniformity, high production rate, and homogeneity in elemental distribution. It is found that with an increase in Al content, the specific capacity decreases but the cyclic stability and rate capability increases. Furthermore, optimum Al-doping not only compensates for the adverse effect of low Co by decreasing the extent of cation mixing, but it also minimizes the electrode polarization and cracking of the particles.

25 ENERGY STORAGE↗
DOE OSTI2020

Synthesis of LiNiO 2 at Moderate Oxygen Pressure and Long-Term Cyclability in Lithium-Ion Full Cells

The widespread adoption of electric vehicles necessitates higher-energy-density and longer-life cathode materials for Li-ion batteries. LiNiO 2 offers a higher energy density at a lower cost than other high-Ni-content cathodes containing additional transition-metal ions. However, detrimental phase transformations and impedance growth, resulting from structural defects formed during synthesis, lead to poor cyclability and limit the practical viability of LiNiO 2 . Herein, we demonstrate a considerably improved cycle life for LiNiO 2 by synthesizing it under a pressurized oxygen environment. The capacity retention in pouch-type full cells with a graphite anode after 1000 cycles is increased from 59 to 76% by applying a mere 1.7 atm of oxygen pressure during the synthesis of LiNiO 2 . With iodometric titration and inductively coupled plasma optical emission spectroscopy analysis, we provide clear evidence that oxygen pressure during synthesis reduces the occurrence of lattice oxygen vacancies and increases the content of Ni 3+ in LiNiO 2 , improving its structural integrity and cyclability. Post-mortem analysis of the cycled cathodes provides insights into the sources of degradation occurring during long-term cycling. Here, this work demonstrates a practically viable, synthetic approach combined with doping and coating to achieve improved performance with high-Ni layered oxide materials. Furthermore, this work represents the first report of extended cycling of LiNiO 2 in pouch full cells with graphite anode and will, therefore, serves as an important benchmark for future research on LiNiO 2 .

25 ENERGY STORAGE↗
NASA NTRS2009

A Study on Advanced Lithium-Based Battery Cell Chemistries to Enhance Lunar Exploration Missions

NASA's Exploration Technology Development Program (ETDP) Energy Storage Project conducted an advanced lithium-based battery chemistry feasibility study to determine the best advanced chemistry to develop for the Altair lunar lander and the Extravehicular Activities (EVA) advanced lunar surface spacesuit. These customers require safe, reliable energy storage systems with extremely high specific energy as compared to today's state-of-the-art batteries. Based on customer requirements, the specific energy goals for the development project are 220 watt-hours per kilogram (Wh/kg) delivered at the battery level at 0 degrees Celsius (degrees Celcius) at a C/10 discharge rate. Continuous discharge rates between C/5 and C/2, operation over 0 to 30 degrees C, and 200 cycles are targeted. The team, consisting of members from NASA Glenn Research Center, Johnson Space Center, and Jet Propulsion laboratory, surveyed the literature, compiled information on recent materials developments, and consulted with other battery experts in the community to identify advanced battery materials that might be capable of achieving the desired results with further development. A variety of electrode materials were considered, including layered metal oxides, spinel oxides, and olivine-type cathode materials, and lithium metal, lithium alloy, and silicon-based composite anode materials. lithium-sulfur systems were also considered. Hypothetical cell constructs that combined compatible anode and cathode materials with suitable electrolytes, separators, current collectors, headers, and cell enclosures were modeled. While some of these advanced materials are projected to obtain the desired electrical performance, there are risks that also factored into the decision making process. The risks include uncertainties due to issues such as safety of a system containing some of these materials, ease of scaling-up of large batches of raw materials, adaptability of the materials to processing using established or reasonable cost manufacturing techniques, manufacturability of the materials in dimensions required for integration into battery cells of practical capacities, low Technology Readiness levels (TRl), and the ability to achieve the desired performance by the customer need dates. The advanced cell chemistry options were evaluated with respect to multiple quantitative and qualitative attributes while considering their projected performance at the end of the available development timeframe. Following a rigorous ranking process, a chemistry that combines a lithiated nickel manganese cobalt oxide (lithium NMC) cathode with a silicon-based composite anode was selected as the technology that can offer the best combination of safety, specific energy, energy density, and likelihood of success. Tasks over the next three years will focus on development of electrode materials, compatible electrolytes, and separator materials, and integration of promising components to assess their combined performance in working cells. Cells of the chosen chemistry will be developed to TRl 6 by 2014 and will then be transferred to the customers for infusion into their mission paths.

Reid, Concha↗
DOE OSTI2025

Assessing the coating implications of slurry formulations in NCMA and LFMP blend cathodes for lithium-ion batteries

This paper investigates the implications of slurry formulations and electrode processing on the performance of lithium-ion battery (LIB) cathodes, focusing on Nickel Cobalt Manganese Aluminum (NCMA) and Lithium Ferro Manganese Phosphate (LFMP) blends. Through a comprehensive examination of electrode processing steps, from material selection to coating application, we elucidate the critical role of processing parameters in shaping electrode morphology and electrochemical behavior. Rheological studies reveal the influence of slurry composition on viscosity and flow behavior, highlighting the importance of achieving optimal rheological properties for uniform coating deposition. Electrochemical characterization, including cyclic voltammetry and rate capability tests, unveils the electrochemical behavior of NCMA, LFMP, and their blend, showcasing the synergistic effects of material blending on battery performance. In conclusion, our findings underscore the intricate relationship between slurry formulation, electrode processing, and LIB performance, offering valuable insights for the design and optimization of high-performance electrode materials for next-generation batteries.

25 ENERGY STORAGE↗
DOE OSTI2021

Li2O-Based Cathode Additives Enabling Prelithiation of Si Anodes

Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li2O) was added to a LiNi0.6Mn0.2Co0.2O2 (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co3O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2O. The Li2O + Co3O4 additives successfully delivered an additional capacity of 1116 mAh/gLi2O when charged up to 4.3 V in half cells and 1035 mAh/gLi2O when charged up to 4.1 V in full cells using Si anodes.

25 ENERGY STORAGE↗
NASA NTRS2014

Development of Large-Format Lithium-Ion Cells with Silicon Anode and Low Flammable Electrolyte

NASA is developing safe, high energy and high capacity lithium-ion cell designs and batteries for future missions under NASAs Advanced Space Power System (ASPS) project. Advanced cell components, such as high specific capacity silicon anodes and low-flammable electrolytes have been developed for improving the cell specific energy and enhancing safety. To advance the technology readiness level, we have developed large-format flight-type hermetically sealed battery cells by incorporating high capacity silicon anodes, commercially available lithium nickel, cobalt, aluminum oxide (NCA) cathodes, and low-flammable electrolytes. In this report, we will present the performance results of these various battery cells. In addition, we will also discuss the post-test cell analysis results as well.

lithium-ion cell↗
DOE OSTI2021

Roles of Mn and Co in Ni-rich layered oxide cathodes synthesized utilizing a Taylor Vortex Reactor

It is reported that layered oxides, composed of nickel, manganese, and cobalt (NMC), are sought after as cathode materials which provide improved energy density, cycle life, and safety in commercial lithium ion batteries (LIBs). Increasing Ni contents higher than 80% can provide even higher practical discharge capacities >200 mAh/g and similar to ~4 V discharge potential vs Li/Li + , making them promising cathodes for next generation LIBs. However, rapid capacity fade during cycling and heat-related safety concerns are delaying their successful transition to industry. We report systematic performance optimization of LiNiO 2 , LiNi 0.9 Mn 0.1 O 2 , and LiNi 0.9 Co 0.1 O 2 high Ni layered oxide cathodes synthesized by utilizing a Taylor Vortex Reactor. Co-free LiNi 0.9 Mn 0.1 O 2 cathode showed 200 mAh/g highest discharge capacity at 0.1 C rate with 84% retention after 103 cycles at 0.3C rate while LiNi 0.9 Co 0.1 O 2 cathode showed higher initial but poor cycle life (225 mAh/g highest discharge capacity at 0.1C rate with only 56% capacity retention after 103 cycles at 0.3 C rate. Synchrotron based X-ray diffraction (SXRD), X-ray absorption spectroscopy (XAS) and focused ion beam (FIB) imaging of pristine and cycled cathodes after 103 cycles provided important information on degradation mechanism. The roles of Mn and Co on layered structure formation, charge balance, cationic mixing, and electrochemical performance were elucidated using the crystallographic information from XRD refinement and electronic state analysis from XAS providing valuable information to design future Ni-rich layered oxide cathodes.

25 ENERGY STORAGE↗
DOE OSTI2021

Temperature-Swing Synthesis of Large-Size Single-Crystal LiNi 0.6 Mn 0.2 Co 0.2 O 2 Cathode Materials

Single-crystal lithium-nickel-manganese-cobalt-oxide (SC-NMC) has recently emerged as a promising battery cathode material due to its outstanding cycle performance and mechanical stability over the tradional polycrystalline NMC. It is favorable to further increase the grain size of SC-NMC particles to achieve a higher volumetric energy density and minimize surface-related degradations. However, the preparation of large-size yet high performance SC-NMC particles faces a challenge in choosing a suitable temperature for sintering. High temperature promotes grain growth but induces cation mixing that negatively impacts the electrochemical performance. Here we report a temperature-swing sintering (TSS) strategy with two isothermal stages that fulfils the needs for grain growth and structural ordering sequentially. A high-temperature sintering is first used for a short period of time to increase grain size and then the reaction temperature is lowered and kept constant for a longer period of time to improve structural ordering and complete the lithiation process. SC-LiNi 0.6 Mn 0.2 Co 0.2 O 2 materials prepared via TSS exhibit large grain size (~4 μm), a low degree of cation mixing (~0.9%), and outperform the control samples prepared by the conventional sintering method. Furthermore, this work highlights the importance of understanding the process-structure-property relationships and may guide the synthesis of other SC Ni-rich cathode materials.

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 OSTI2024

Chemo-Mechanical Instabilities in Lithium Cobalt Oxide at Higher State-Of-Charge in Li-Ion Batteries

Transition metal oxide cathodes are widely used in commercial Li-ion batteries. However, their practical charge capacity is limited due to severe chemo-mechanical instabilities at higher charge voltage, and state-of-charge condition. Here, in situ stress and strain measurements were synchronized to probe mechanical deformations in the lithium cobalt oxide (LCO) cathode via a multi-beam stress sensor and digital image correlation, respectively. In situ mechanical measurements revealed how Li removal from the electrode structure induces deformations on the LCO composite cathodes during cycling. The structure and morphology of the LCO cathodes were further investigated by X-ray diffraction (XRD) and scanning electron microscopy (SEM) studies. Two distinct electrochemical and mechanical behaviors were identified when the LCO was charged up to 4.65 V. The LCO undergoes a compressive stress generation when charged up to 4.2 V and surface fractures on the LCO particles were detected by SEM. LCO cathode experienced significantly large contractions (negative strains) when charged up to 4.65 V, where intergranular crack formation and phase transformation were detected on the LCO particles via SEM and XRD, respectively. Overall, the study bridges complicated structural deformations with in situ analysis of mechanical degradations in LCO cathodes charged at higher voltages. The correlation is vital to understanding instability mechanisms in transition metal oxides at high voltages for alkali metal ion batteries.

higher state-of-charge↗
DOE OSTI2024

Low-cost iron trichloride cathode for all-solid-state lithium-ion batteries

The dominant chemistries of lithium-ion batteries on the market today still rely on flammable organic liquid electrolytes and cathodes containing scarce metals, such as cobalt or nickel, raising safety, cost and environmental concerns. Here we show a FeCl 3 cathode that costs as little as 1% of the cost of a LiCoO 2 cathode or 2% of a LiFePO 4 cathode. Once coupled with a solid halide electrolyte and a lithium-indium (Li–In) alloy anode, it enables all-solid-state lithium-ion batteries without any liquid components. Notably, FeCl 3 exhibits two flat voltage plateaux between 3.5 and 3.8 V versus Li + /Li, and the solid cell retains 83% of its initial capacity after 1,000 cycles with an average Coulombic efficiency of 99.95%. Combined neutron diffraction and X-ray absorption spectroscopy characterizations reveal a Li-ion (de)intercalation mechanism together with a Fe 2+ /Fe 3+ redox process. Further, our work provides a promising avenue for developing sustainable battery technologies with a favourable balance of performance, cost and safety.

25 ENERGY STORAGE↗
DOE OSTI2023

Direct recycling of spent nickel-rich cathodes in reciprocal ternary molten salts

Lithium-ion batteries (LIBs) have revolutionized portable electronics and electric vehicles (EVs), but the growing accumulation of end-of-life (EOL) batteries poses environmental challenges. Recycling high-value cathodes from EOL LIBs can minimize waste and reduce the need for mining critical minerals. Here, this study focuses on the direct recycling of Ni-rich cathodes, particularly lithium-manganese-cobalt-oxide (NMC) 622 in a “reciprocal ternary molten salts (RTMS)" system. The ionothermal relithiation in the RTMS system successfully restores the layered structure, lithium content, and electrochemical performance of the NMC 622 cathode, comparable to the pristine material. The cost analysis reveals that cathode regeneration through ionothermal relithiation is more economical than virgin production or conventional recycling methods.

25 ENERGY STORAGE↗
NASA NTRS2010

A Study on Advanced Lithium-Based Battery Cell Chemistries to Enhance Lunar Exploration Missions

NASAs Exploration Technology Development Program (ETDP) Energy Storage Project conducted an advanced lithium-based battery chemistry feasibility study to determine the best advanced chemistry to develop for the Altair Lunar Lander and the Extravehicular Activities (EVA) advanced Lunar surface spacesuit. These customers require safe, reliable batteries with extremely high specific energy as compared to state-of-the-art. The specific energy goals for the development project are 220 watt-hours per kilogram (Wh/kg) delivered at the battery-level at 0 degrees Celsius ( C) at a C/10 discharge rate. Continuous discharge rates between C/5 and C/2, operation between 0 and 30 C and 200 cycles are targeted. Electrode materials that were considered include layered metal oxides, spinel oxides, and olivine-type cathode materials, and lithium metal, lithium alloy, and silicon-based composite anode materials. Advanced cell chemistry options were evaluated with respect to multiple quantitative and qualitative attributes while considering their projected performance at the end of the available development timeframe. Following a rigorous ranking process, a chemistry that combines a lithiated nickel manganese cobalt oxide Li(LiNMC)O2 cathode with a silicon-based composite anode was selected as the technology that can potentially offer the best combination of safety, specific energy, energy density, and likelihood of success.

Reid, Concha M.↗
DOE OSTI2025

Reciprocal Ternary Molten Salts Enable the Direct Upcycling of Spent Lithium‐Nickel‐Manganese‐Cobalt Oxide (NMC) Mixtures to Make NMC 622

Cathode active material is the most valuable component of spent lithium‐ion batteries, accounting for ≈30% of their overall value. Direct recycling of cathode materials involves recovering, regenerating, and reusing them without breaking down their chemical structure. This approach maximizes the added value of the cathode compound and reduces manufacturing costs by avoiding the need for virgin material production. However, one key challenge in scaling direct recycling from lab to industry is the requirement for highly purified cathode materials, contrasting with the low purity of black mass generated from battery shredding. No efficient separation process currently exists to isolate different lithium‐nickel‐manganese‐cobalt oxides (NMCs) from each other. Thus, direct recycling technologies that can operate with mixtures of multiple NMC stoichiometries will be best‐suited for industrial adoption. This study explores the direct recycling of NMC mixtures into NMC 622 using a “reciprocal ternary molten salts (RTMS)” system. Ionothermal relithiation and upcycling within the RTMS system successfully restore the layered structure, lithium content, and electrochemical performance of degraded NMCs, yielding results comparable to pristine NMC 622 (P‐NMC 622).

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 OSTI2020

Perspectives on the relationship between materials chemistry and roll-to-roll electrode manufacturing for high-energy lithium-ion batteries

As lithium-ion battery (LIB) active material and cell manufacturing costs continue to drop with wider adoption of electric vehicles, electrode and cell processing costs remain too high in terms of reaching the ultimate U.S. Department of Energy (DOE) cell cost target of $80/kWh. This paper primarily covers major materials chemistry advancements made over the last 10 years at Oak Ridge National Laboratory (ORNL) in the space of advanced manufacturing science for LIBs with the aim of simultaneously meeting the ultimate cost target, 500 Wh/kg gravimetric energy density, 10-15-min fast charge times, and 1000 deep discharge cycles. Aqeous electrode processing with a variety of active anode and cathode materials is now a standard procedure at the DOE Battery Manufacturing R&D Facility at ORNL (BMF), including the latest processes developed for Ni-rich cathodes. New results on cobalt-free LiNi 0.8 Fe 0.1 Al 0.1 O 2 (NFA 811) are also included and discussed in an electrode processing advantage context. In addition, colloidal processing advancements have been made for Si/C composite anodes for achieving >600 mA h/g capacities. Optimization of electrode coating parameters and drying protocols have been completed, which has elucidated how key processing variables need to be changed when parameters such as slurry solids loading, solvent type, and wet electrode thickness are changed. ORNL has also increased the line speeds at which thick cathodes can be processed using ultra-fast electron beam (EB) curing and substantially decreased formation cycling times to <1 day. Finally, key details of these advancements are discussed in the context of materials chemistry and process-property-performance relationships.

25 ENERGY STORAGE↗