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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Relithiation process for direct regeneration of cathode materials from spent lithium-ion batteries

A method for the regeneration of cathode material from spent lithium-ion batteries is provided. The method includes dissolving a lithium precursor in a polyhydric alcohol to form a solution. Degraded cathode material containing lithium metal oxides are dispersed into the solution under mechanical stirring, forming a mixture. The mixture is heat treated within a reactor vessel or microwave oven. During this heat treatment, lithium is intercalated into the degraded cathode material. The relithiated electrode material is collected by filtration, washing with solvents, and drying. The relithiated electrode material is then ground with a lithium precursor and thermally treated at a relatively low temperature for a predetermined time period to obtain regenerated cathode material.

Belharouak, Ilias↗
DOE OSTI2024

Manganese-rich high entropy oxides for lithium-ion batteries:materials design approaches to address voltage fade

Lithium- and manganese-rich oxides are of interest as lithium-ion battery cathode materials as Mn is earth abundant, low cost, and can deliver high capacity. Herein, a high entropy strategy was used to prepare Mn rich high entropy oxide (HEO) materials by including four additional metals (Ni, Co, Fe and Al) in the compositions using a mild co-precipitation method. Two HEOs (Li x Ni 0.1 Mn 0.6 Co 0.1 Al 0.1 Fe 0.1 O y , where x = 1.5 for HEO-L and x = 0.5 for HEO-H) with layered and spinel-layered hybrid structures were investigated where the morphology, elemental composition, structure, atomic level phase distribution, and electrochemistry were determined. The HEO-L samples involve a Li 2 TMO 3 layered structure with ~39% stacking faults. HEO-H is a hybrid structure comprised of 80 wt% spinel and 20 wt% LiMO 2 layered structure. The high entropy manganese-rich HEO-L showed higher capacity and 93% retention of the average voltage after 100 cycles while HEO-H showed higher capacity retention and near 100% average voltage retention. Finally, operando X-ray absorption spectroscopy revealed that the Ni, Co, and Mn are redox active in both materials while the Fe center remains at the Fe 3+ oxidation state throughout cycling, where the changes in the oxidation states for both materials during discharge were consistent with the delivered electrochemical capacity rationalizing the observed electrochemistry.

25 ENERGY STORAGE↗
DOE OSTI2020

Improved Capacity Retention of Lithium Ion Batteries under Fast Charge via Metal-Coated Graphite Electrodes

A primary barrier preventing repetitive fast charging of Li-ion batteries is lithium metal plating at the graphite anode. One approach toward mitigating Li metal deposition is the deliberate modification of the graphite anode surface with materials demonstrating high overpotentials unfavorable for Li metal nucleation, such as Ni or Cu nanoscale films. This research explores Ni and Cu surface coatings at different areal loadings (3 or 11 μg cm -2 ) on the electrochemistry of graphite/LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) type Li-ion batteries. Extended galvanostatic cycling of control and metal-coated electrodes in graphite/NMC622 pouch cells are conducted under high rate conditions. Based on the overpotential of Li deposition on metal foil, both Ni and Cu treatments were anticipated to result in reduced lithium deposition. The higher metal film loadings of 11 μg cm -2 Ni- or Cu-coated electrodes exhibit the highest capacity retention after 500 cycles, with mean improvements of 8% and 9%, respectively, over uncoated graphite electrodes. Li plating quantified by X-ray diffraction indicates that the metal films effectively reduce the quantity of plated Li compared to untreated electrodes, with 11 μg cm -2 Cu providing the greatest benefit.

25 ENERGY STORAGE↗
DOE OSTI2022

Decomposition of PVDF to delaminate cathode materials from end-of-life lithium-ion battery cathodes

The growing demand of electric vehicles and rapid consumption of rechargeable lithium-ion batteries (LIBs) require recycling of spent cathode active materials (CAMs) to reduce hazardous wastes and supply raw materials to LIB production. To separate CAMs from the cathode, direct calcination of polyvinylidene fluoride (PVDF) binder is widely applied, which leads to high energy consumption and release of toxic hydrogen fluoride. It is desirable to have an environmentally friendly and effective alternative to traditional direct calcination. In this study, five lithium salts, LiOAc (lithium acetate), LiNO 3 , LiCl, Li 2 CO 3 , and Li 2 SO 4 , were deployed and compared for their performance in recycling CAMs. A peel-off efficiency of up to 98.5% was achieved at a LiOAc to LiNO 3 molar ratio of 3:2, salt to cathode mass ratio of 10:1, and temperature of 300 °C at a holding time of 30 min. This system avoids corrosive chemicals and minimizes particle agglomeration of recycled products. Compared with sodium salt systems (NaOAc-NaNO 3 ) or direct calcination, the LiOAc-LiNO 3 system prevented high reaction temperature or further lithium loss and minimized crystal structure and morphological changes. In conclusion, a decomposition mechanism of PVDF through adsorption of HF and fluorine substitution was proposed.

25 ENERGY STORAGE↗
DOE OSTI2020

Enhancing nanostructured nickel-rich lithium-ion battery cathodes via surface stabilization

Layered, nickel-rich lithium transition metal oxides have emerged as leading candidates for lithium-ion battery (LIB) cathode materials. High-performance applications for nickel-rich cathodes, such as electric vehicles and grid-level energy storage, demand electrodes that deliver high power without compromising cell lifetimes or impedance. Nanoparticle-based nickel-rich cathodes seemingly present a solution to this challenge due to shorter lithium-ion diffusion lengths compared to incumbent micrometer-scale active material particles. However, since smaller particle sizes imply that surface effects become increasingly important, particle surface chemistry must be well characterized and controlled to achieve robust electrochemical properties. Moreover, residual surface impurities can disrupt commonly used carbon coating schemes, which result in compromised cell performance. Using x-ray photoelectron spectroscopy, here we present a detailed characterization of the surface chemistry of LiNi0.8Al0.15Co0.05O2 (NCA) nanoparticles, ultimately identifying surface impurities that limit LIB performance. With this chemical insight, annealing procedures are developed that minimize these surface impurities, thus improving electrochemical properties and enabling conformal graphene coatings that reduce cell impedance, maximize electrode packing density, and enhance cell lifetime fourfold. Overall, this work demonstrates that controlling and stabilizing surface chemistry enables the full potential of nanostructured nickel-rich cathodes to be realized in high-performance LIB technology.

Lim, Jin-Myoung↗
DOE OSTI2021

MnSn 2 and MnSn 2 –TiO 2 nanostructured anode materials for lithium-ion batteries

The high theoretical lithium storage capacity of Sn makes it an enticing anode material for Li-ion batteries (LIBs); however, its large volumetric expansion during Li–Sn alloying must be addressed. Combining Sn with metals that are electrochemically inactive to lithium leads to intermetallics that can alleviate volumetric expansion issues and still enable high capacity. Here, we present the cycling behavior of a nanostructured MnSn 2 intermetallic used in LIBs. Nanostructured MnSn 2 is synthesized by reducing Sn and Mn salts using a hot injection method. The resulting MnSn 2 is characterized by x-ray diffraction and transmission electron microscopy and then is investigated as an anode for LIBs. The MnSn 2 electrode delivers a stable capacity of 514 mAh g -1 after 100 cycles at a C/10 current rate with a Coulombic efficiency >99%. Unlike other Sn-intermetallic anodes, an activation overpotential peak near 0.9 V versus Li is present from the second lithiation and in subsequent cycles. We hypothesize that this effect is likely due to electrolyte reactions with segregated Mn from MnSn 2 . To prevent these undesirable Mn reactions with the electrolyte, a 5 nm TiO 2 protection layer is applied onto the MnSn 2 electrode surface via atomic layer deposition. The TiO 2 -coated MnSn 2 electrodes do not exhibit the activation overpotential peak. The protection layer also increases the capacity to 612 mAh g -1 after 100 cycles at a C/10 current rate with a Coulombic efficiency >99%. This higher capacity is achieved by suppressing the parasitic reaction of Mn with the electrolyte, as is supported by x-ray photoelectron spectroscopy analysis.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Methods for the production of cathode materials for lithium ion batteries

The present disclosure provides methods for producing cathode materials for lithium ion batteries. Cathode materials that contain manganese are emphasized. Representative materials include LixNi1-y-zMnyCozO2 (NMC) (where x is in the range from 0.80 to 1.3, y is in the range from 0.01 to 0.5, and z is in the range from 0.01 to 0.5), LixMn2O4 (LM), and LixMn2-yNiyO2 (LMN) (where x is in the range from 0.8 to 1.3 and y is in the range from 0.0 to 0.8). The process includes reactions of carboxylate precursors of nickel, manganese, and/or cobalt and lithiation with a lithium precursor. The carboxylate precursors are made from reactions of pure metals or metal compounds with carboxylic acids. The manganese precursor contains bivalent manganese and the process controls the oxidation state of manganese to avoid formation of higher oxidation states of manganese.

Huang, Baoquan↗
DOE OSTI2023

Methods for the production of cathode materials for lithium ion batteries

The present disclosure provides methods for producing cathode materials for lithium ion batteries. Cathode materials that contain manganese are emphasized. Representative materials include Li x Ni 1−y−z Mn y Co z O 2 (NMC) (where x is in the range from 0.80 to 1.3, y is in the range from 0.01 to 0.5, and z is in the range from 0.01 to 0.5), Li x Mn 2 O 4 (LM), and Li x Ni 1−y Mn y O 2 (LMN) (where x is in the range from 0.8 to 1.3 and y is in the range from 0.0 to 0.8). The process includes reactions of carboxylate precursors of nickel, manganese, and/or cobalt and lithiation with a lithium precursor. The carboxylate precursors are made from reactions of pure metals or metal compounds with carboxylic acids. The manganese precursor contains bivalent manganese and the process controls the oxidation state of manganese to avoid formation of higher oxidation states of manganese.

Huang, Baoquan↗
DOE OSTI2022

Methods for the production of cathode materials for lithium ion batteries

The present disclosure provides methods for producing cathode materials for lithium ion batteries. Cathode materials that contain manganese are emphasized. Representative materials include Li x Ni 1-y-z Mn y Co z O 2M (NMC) (where x is in the range from 0.80 to 1.3, y is in the range from 0.01 to 0.5, and z is in the range from 0.01 to 0.5), Li x Mn 2 O 4 (LM), and Li x Ni 1-y Mn y O 2 (LMN) (where x is in the range from 0.8 to 1.3 and y is in the range from 0.0 to 0.8). The process includes reactions of carboxylate precursors of nickel, manganese, and/or cobalt and lithiation with a lithium precursor. The carboxylate precursors are made from reactions of pure metals or metal compounds with carboxylic acids. The manganese precursor contains bivalent manganese and the process controls the oxidation state of manganese to avoid formation of higher oxidation states of manganese.

Huang, Baoquan↗
DOE OSTI2020

Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries

The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li ion batteries. Several lithium chloride SEs, Li 3 MCl 6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li 3 MCl 6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li 3 MCl 6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, TI, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li 3 MCl 6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M 3+ with Zr 4+ . Zr-substituted phase (Li 2.5 M 0.5 Zr 0.5 Cl 6 , M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li 3 MCl 6 SEs could lead to superionic Li 3 MCl 6 SEs.

25 ENERGY STORAGE↗
DOE OSTI2023

Ionothermally Synthesized Nanoporous Ti 0.95 W 0.05 Nb 2 O 7 : a Novel Anode Material for High-Performance Lithium-Ion Batteries

Although TiNb 2 O 7 is regarded as a fast-rechargeable lithium-ion battery (LIB) anode material, the intrinsic poor electrochemical kinetics of TiNb 2 O 7 still dramatically impedes its development. Herein, an ionothermal synthesis-assisted doping strategy is proposed for the preparation of a new W 6+ -doped TiNb 2 O 7 material (Ti 0.95 W 0.05 Nb 2 O 7 ) with nanoporous structure (denoted as NPTWNO). The improved Li + diffusion coefficient of NPTWNO suggests that the ionic-liquid-templated nanoporous architecture improves the Li+ diffusion kinetics. The density functional theory computational study reveals that the doped W 6+ successfully boosts the electronic conductivity due to the narrowed conduction-valance bandgap resulted from charge redistribution, which is reflected by the electrochemical impedance spectroscopy data. With the simultaneously enhanced Li+ diffusivity and electronic conductivity, NPTWNO achieves fast-rechargeability in LIBs. So this work indicates the potential of ionothermal synthesis-assisted doping strategy on energy storage materials and offers NPTWNO material with promising electrochemical performance.

25 ENERGY STORAGE↗
DOE OSTI2023

A conformal heat-drying direct ink writing 3D printing for high-performance lithium-ion batteries

High areal capacity electrodes hold great potential for high-energy density lithium-ion batteries (LIBs), but their poor electrochemical kinetics limit their power density. Here, in this study, high areal capacity 3D-structured LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathodes (4.3 mAh cm -2 ) are prepared via 3D printing with a manner of direct ink writing. The electrodes had an enlarged electrode–electrolyte contact area, shortened diffusion pathway, and reduced intercalation-induced stress, thereby delivering enhanced rate capability and cyclability in LIBs, which is 143.6 mAh g -1 at 3C and a 60.2 % capacity retention over 800 cycles at 1C. Moreover, at electrode level, the 3D-NMC exhibits an energy and power densities of 313.1 Wh kg -1 and 657.9 W kg -1 , respectively. Furthermore, the theoretical calculation suggests that reducing the gap width will be highly beneficial to the energy and power densities. This work establishes a milestone in understanding the cycling effect on the electrode local structure, including the void area and the LiNi 0.8 Mn 0.1 Co 0.1 O 2 region, which confirms the effectiveness of 3D printing for electrode preparation.

25 ENERGY STORAGE↗
DOE OSTI2023

Pitch Carbon-coated Ultrasmall Si Nanoparticle Lithium-ion Battery Anodes Exhibiting Reduced Reactivity with Carbonate-based Electrolyte

Silicon anodes for lithium-ion batteries (LIBs) have the potential for higher energy density compared to conventionally used graphite-based LIB anodes. However, silicon anodes exhibit poor cycle and calendar lifetimes due to mechanical instabilities and high chemical and electrochemical reactivity with the carbonate-based electrolytes that are typically used in LIBs. In this work, we synthesize a pitch carbon-coated silicon nanoparticle composite active material for LIB anodes that exhibits reduced chemical reactivity with carbonate-based electrolytes compared to an uncoated silicon anode. Silicon primary particle sizes less than 10 nm diameter minimize micro-scale mechanical degradation of the anode composite, while conformal coatings of pitch carbon minimize the parasitic reactions between the silicon and the electrolyte. When matched with a high voltage NMC622 (LiNi 0.6 Mn 0.2 Co 0.2 O 2 ) cathode, the pitch carbon-coated silicon anode retains approximately 75% of its initial capacity at the end of 1000 cycles. Increasing the areal loading of the pitch carbon-coated silicon anodes to realize energy density improvements over graphite anodes results in severe mechanical degradation on the electrode level, highlighting a remaining challenge to be addressed in future work.

25 ENERGY STORAGE↗
DOE OSTI2021

New Insights into the High‐Performance Black Phosphorus Anode for Lithium‐Ion Batteries

Abstract Black phosphorus (BP) is a promising anode material in lithium‐ion batteries (LIBs) owing to its high electrical conductivity and capacity. However, the huge volume change of BP during cycling induces rapid capacity fading. In addition, the unclear electrochemical mechanism of BP hinders the development of rational designs and preparation of high‐performance BP‐based anodes. Here, a high‐performance nanostructured BP–graphite–carbon nanotubes composite (BP/G/CNTs) synthesized using ball‐milling method is reported. The BP/G/CNTs anode delivers a high initial capacity of 1375 mA h g −1 at 0.15 A g −1 and maintains 1031.7 mA h g −1 after 450 cycles. Excellent high‐rate performance is demonstrated with a capacity of 508.1 mA h g −1 after 3000 cycles at 2 A g −1 . Moreover, for the first time, direct evidence is provided experimentally to present the electrochemical mechanism of BP anodes with three‐step lithiation and delithiation using ex situ X‐ray diffraction (XRD), ex situ X‐ray absorption spectroscopy (XAS), ex situ X‐ray emission spectroscopy, operando XRD, and operando XAS, which reveal the formation of Li 3 P 7 , LiP, and Li 3 P. Furthermore, the study indicates an open‐circuit relaxation effect of the electrode with ex situ and operando XAS analyses.

Li, Minsi↗
DOE OSTI2025

Amorphous zinc–molybdenum–sulfide chalcogel as a long-cycle, high-capacity electrode for lithium-ion batteries

The inherent limitations of intercalation-based electrodes in lithium-ion batteries have prompted the search for alternative materials with higher specific capacities and robust electrochemical stability. Sulfur-based electrodes, despite their high theoretical capacities (1672 mAh g −1 ), typically suffer from poor cycling performance. In this work, zinc molybdenum polysulfide (Zn x Mo 3 S 13 , 0.5 ≤ x), an amorphous semiconductor chalcogel, exhibits high specific capacity and excellent cycling stability. Synchrotron X-ray pair distribution function and extended X-ray absorption fine structure analyses reveal a short-range atomic structure comprising Mo–Mo, M–S (M = Mo, Zn), and S–S bonding motifs. The coordination environment of Mo and S closely resembles that of Mo 3 S 13 clusters, interconnected via S–S bridges and Zn 2+ cations. The Li/Zn x Mo 3 S 13 cell delivers an initial discharge capacity of 844 mAh g −1 at C/3, and retains 386.2 mAh g −1 after 1000 cycles with an average coulombic efficiency of 99.99%. The distribution of relaxation times analysis confirms the formation of a stable solid electrolyte interphase, which underpins the cell's long-term stability. In conclusion, this outstanding performance is attributed to the synergistic effects of the chalcogel's unique amorphous framework, semiconductive character, Zn-mediated polysulfide anchoring, and structural resilience, positioning Zn x Mo 3 S 13 chalcogel among the most durable pure metal sulfide cathodes reported for next-generation LIBs.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Identification and characterization of the dominant thermal resistance in lithium-ion batteries using operando 3-omega sensors

Poor thermal transport within lithium-ion batteries fundamentally limits their performance, safety, and lifetime, in spite of external thermal management systems. All prior efforts to understand the origin of batteries' mysteriously high thermal resistance have been confined to ex situ measurements without understanding the impact of battery operation. Here, we develop a frequency-domain technique that employs sensors capable of measuring spatially resolved intrinsic thermal transport properties within a live battery while it is undergoing cycling. Our results reveal that the poor battery thermal transport is due to high thermal contact resistance between the separator and both electrode layers and worsens as a result of formation cycling, degrading total battery thermal transport by up to 70%. We develop a thermal model of these contact resistances to explain their origin. These contacts account for up to 65% of the total thermal resistance inside the battery, leading to far-reaching consequences for the thermal design of batteries. Finally, our technique unlocks new thermal measurement capabilities for future battery research.

25 ENERGY STORAGE↗
NASA NTRS2000

Engineering and Abuse Testing of Panasonic Lithium-Ion Battery and Cells

This viewgraph presentation reviews the performance testing of Lithium Ion batteries and cells under different conditions of charge and discharge. The tests show that the 0.5 C rate of charge and discharge might be the ideal condition for long term cycling. It reviews the issues of overcharge and overdischarge of the cells. The cells and the battery have adequate protection under both conditions to prevent any catastrophic occurrences. Temperatures above 150 C are required to vent the cells or cause a thermal runaway, Since this situation is non-credible in the cabin of the Space Shuffle or ISS this should not pose a problem. The presentation includes graphs and charts showing the charge and discharge capacities of the battery and also the current and voltage profiles. A view of a circuit board which contains the controlling mechanism for the battery is also shown.

Jeevarajan, Judith A.↗
DOE OSTI2020

Improved methods for separation of Cobalt, Manganese, Nickel, Lithium from Waste Lithium-ion Battery Scrap

Improved methods for separation of Cobalt, Manganese, Nickel, Lithium from Waste Lithium-ion Battery Scrap Mark L. Strauss1, John Klaehn1 Luis Diaz Aldana1, Tedd Lister1 Idaho National Laboratory1, Biological and Chemical Processing Department, Idaho Falls, Idaho 83415 ABSTRACT The current methods for the separation of Co, Mn, Ni, Li require that the leach solution have a pH between 2-4 in order to use many Cyanex cationic exchange products. Using a unique buffer solution for the reagent combined with the leachate of innovative electrochemical leaching process for lithium batteries demonstrates the separation is possible without a large of pH modification as other commercial hydrometallugical separation process. This research demonstrates a process that is more environmentally sustainable because the reagent consumption may be less. The corresponding McCable-Thiele diagrams and number of theoretical stages were determined to achieve a 80-90% purity of cobalt, manganese, nickel and lithium.

42 ENGINEERING↗