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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Suppressing Universal Cathode Crossover in High‐Energy Lithium Metal Batteries via a Versatile Interlayer Design**

Abstract The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high‐energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as‐induced dual‐gradient solid‐electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm −2 . Moreover, X‐ray photoelectron spectroscopy and synchrotron X‐ray experiments revealed that N‐rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high‐energy cathode materials including LiNi 0.7 Mn 0.2 Co 0.1 O 2 , Li 1.2 Co 0.1 Mn 0.55 Ni 0.15 O 2 , and sulfur demonstrate significantly improved cycling stability with high cathode loading.

Xie, Chuyi↗
DOE OSTI2021

Optimization of Magnesium-Doped Lithium Metal Anode for High Performance Lithium Metal Batteries through Modeling and Experiment

Lithium (Li)-magnesium (Mg) alloy with limited Mg amount, which can also be called Mg-doped Li (Li-Mg), has been considered as a potential alternative anode for high energy density rechargeable Li metal batteries. However, the optimum doping-content of Mg in Li-Mg anode and the mechanism of the improved performance are not well understood. In this study, density functional theory (DFT) calculations are used to investigate the effect of Mg amount in Li-Mg anode. The Li-Mg with about 5 wt. % Mg (abbreviated as Li-Mg5) has the lowest absorption energy of Li, thus all the surface area can be “controlled” by Mg atoms, leading to the smooth and continuous deposition of Li on the surface around the Mg center. A localized high concentration electrolyte enables Li-Mg5 to exhibit the best cycling stability in Li metal batteries with high-loading cathode and lean electrolyte under 4.4 V high-voltage, which is approaching the demand of practical application. This electrolyte also helps generate an inorganic-rich solid electrolyte interphase, which leads to smooth, compact and less corrosion layer on the Li-Mg5 surface. Both theoretical simulations and experimental results prove that Li-Mg5 has optimum Mg content and gives best battery cycling performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Suppressing Universal Cathode Crossover in High‐Energy Lithium Metal Batteries via a Versatile Interlayer Design**

Abstract The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high‐energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as‐induced dual‐gradient solid‐electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm −2 . Moreover, X‐ray photoelectron spectroscopy and synchrotron X‐ray experiments revealed that N‐rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high‐energy cathode materials including LiNi 0.7 Mn 0.2 Co 0.1 O 2 , Li 1.2 Co 0.1 Mn 0.55 Ni 0.15 O 2 , and sulfur demonstrate significantly improved cycling stability with high cathode loading.

25 ENERGY STORAGE↗
DOE OSTI2024

Ameliorating the sodium storage performance of hard carbon anode through rational modulation of binder

Hard carbon anodes have emerged as promising candidates for sodium-ion batteries due to their inherent advantages. Nevertheless, the surface imperfections in these materials often culminate in irreversible electrolyte consumption, fostering the development of a heterogeneous and fragile solid electrolyte interface (SEI), thereby compromising the initial Coulombic efficiency (ICE). Here, drawing inspiration from the catalytic potential of C=O (carbonyl) bonds in directing preferential salt reduction, we introduce a novel strategy that leverages the modulation of the binder, a long-term overlooked pivotal components in the electrode process. Specifically, Polymethyl methacrylate (PMMA), abundant in C=O groups, is partially substituted for PVDF, ensuring robust adhesion of the electrode material to the current collector while preserving superior mechanical properties. The accurate combination of two binders with delightful compatibility in the state-of-art electrode process, can promote a uniform formation of the SEI on the hard carbon surface enriched in inorganic components, which can ensure long-term interfacial stability and suppresses excessive solvent decomposition and facilitates Na + transfer at the interface. Consequently, the initial Coulombic efficiency of the hard carbon anode with 70 %PMMA binder achieves 86 %, with prominent cycling stability (88 % capacity retention over 500 cycles) at a high current density of 1.2 A g −1 . When paired with high loading cathodes to assemble the pouch cell, it also demonstrates stable operational scenarios.

25 ENERGY STORAGE↗
DOE OSTI2019

Enabling High-Voltage Lithium-Metal Batteries under Practical Conditions

Rechargeable lithium (Li) metal batteries (LMBs) offer a great opportunity for applications needing high-energy-density battery systems. However, rare progress has been demonstrated so far under practical conditions including high voltage, high loading cathode, thin Li anode, and lean electrolyte. Here, in opposite to the common wisdom, we report an ether-based localized high concentration electrolyte that can greatly enhance the stability of Ni-rich LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode under 4.4 V and 4.5 V with an effective protection interphase enriched in LiF. This effect, in combination with the superior Li stability in this electrolyte, enables dramatically improved cycling performances of Li||NMC811 batteries under highly challenging conditions. The LMBs can retain over 80% capacity in 150 stable cycles with extremely limited amounts of Li anode and electrolyte. The findings in this work point out a very promising strategy to develop practical high-energy LMBs.

Ren, Xiaodi↗
DOE OSTI2018

Lithium-ion conductive ceramic textile: A new architecture for flexible solid-state lithium metal batteries

Designing solid-state lithium metal batteries requires fast lithium-ion conductors, good electrochemical stability, and scalable processing approaches to device integration. In this work, we demonstrate a unique design for a flexible lithium-ion conducting ceramic textile with the above features for use in solid-state batteries. The ceramic textile was based on the garnet-type conductor Li 7 La 3 Zr 2 O 12 and exhibited a range of desirable chemical and structural properties, including: lithium-ion conducting cubic structure, low density, multi-scale porosity, high surface area/volume ratio, and good flexibility. The solid garnet textile enabled reinforcement of a solid polymer electrolyte to achieve high lithium-ion conductivity and stable long-term Li cycling over 500 h without failure. The textile also provided an electrolyte framework when designing a 3D electrode to realize ultrahigh cathode loading (10.8 g/cm 2 sulfur) for high-performance Li-metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries

Nanostructured carbon host materials are widely used to improve both sulfur utilization rate and reaction kinetics in lithium-sulfur (Li-S) batteries. However, high complexity/cost of materials synthesis and difficulty in processing nano-materials into high-mass-loading electrodes are still significant barriers to the development of low-cost and high-energy Li-S batteries. In this study, we reported a generic and scalable synthesis approach to prepare nitrogen-doped secondary carbon particles. By using nitrogen-containing precursor as an integration reagent, the nanosized Ketjen Black particles were integrated into micron-size secondary ones and nitrogen-doped (NKB) simultaneously through a one-step heat treatment. With NKB as an example material, the effects of particle integration degree on the secondary particles’ structures, pore volume and connectivity, sulfur loading capability, and cell performance were studied and discussed. At an optimal integration condition, the NKB particles had significantly improved particle dimensions with well-maintained high specific surface area and pore volume. Here, contributed by the micron size and high pore volume, the NKB/S were successfully used for high-sulfur-loading cathodes (4–7 mg s /cm -2 ) and were able to deliver a specific capacity of ~1100 mAh g -1 at a low-porosity (50%) and lean-electrolyte conditions (E/S =4 µL/mg -1 ). Feasibility of the materials for practical use was validated through scaling up synthesis (40 g/batch), large-area electrode coating, and practical pouch cell (1.6 Ah) assembly and test.

25 ENERGY STORAGE↗
DOE OSTI2019

High-Concentration Ether Electrolytes for Stable High-Voltage Lithium Metal Batteries

High-voltage (>4.0 V) rechargeable lithium (Li) metal batteries face huge obstacles due to the high reactivity of Li metal with traditional organic carbonate electrolytes. It is generally accepted that ether-based electrolytes are unstable above 4.0 V and thus unsuitable for high voltage applications, despite of their good compatibility with Li metal. Here we report a concentrated ether electrolyte that could be used under high voltage up to 4.5 V with the formation of a unique cathode/electrolyte interphase enriched in LiF, which effectively preserves the cathode crystalline structural integrity. Employing this high concentration ether electrolyte, Li metal batteries with a moderately high cathode loading of 1.5 mAh cm-2 can have a capacity retention of 92% after 500 cycles at 4.3 V and demonstrate nearly 100% cycling efficiency even at 4.5 V.

Ether, electrolyte, high voltage, stability, lithi↗
DOE OSTI2022

High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes

All-solid-state Li batteries (ASSBs) employing inorganic solid electrolytes offer improved safety and are exciting candidates for next-generation energy storage. Herein, we report a family of lithium mixed-metal chlorospinels, Li 2 In x Sc 0.666-x Cl 4 (0 ≤ x ≤ 0.666), with high ionic conductivity (up to 2.0 mS cm -1 ) owing to a highly disordered Li-ion distribution, and low electronic conductivity (4.7 × 10-10 S cm -1 ), which are implemented for high-performance ASSBs. Owing to the excellent interfacial stability of the SE against uncoated high-voltage cathode materials, ASSBs utilizing LiCoO 2 or LiNi 0.85 Co 0.1 Mn 0.05 O 2 exhibit superior rate capability and long-term cycling (up to 4.8 V versus Li+/Li) compared to state-of-the-art ASSBs. In particular, the ASSB with LiNi 0.85 Co 0.1 Mn 0.05 O 2 exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. Additionally, high cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm -2 (~190 mAh g -1 ).

25 ENERGY STORAGE↗
DOE OSTI2019

Self-Smoothing Anode for Achieving High-Energy Lithium Metal Batteries under Realistic Conditions

Solving the lithium (Li) metal problem is one of the most significant challenges for future high energy batteries. Despite significant efforts to stabilize Li-metal anode structures and prevent dendrite formation, achieving long cycling life in high energy cells remains extremely difficult due to a combination of complex failure modes involving accelerated anode degradation, and depletion of the electrolyte and the Li metal. Here, we report a stable and self-smoothing Li anode structure based on amine-functionalized three-dimensional (3D) carbon fibers for long-cycling life full cells under conditions required for high energy, rechargeable Li-metal batteries. Reversible and smooth Li deposition and stripping is realized on the new anode structure, in contrast with the porous and dendritic Li layers that develop on a pure Li-metal surface. The stable, self-smoothing anode coupled with high-capacity LiNi0.8Mn0.1Co0.1O2 delivers stable cycling using parameters for a high energy cell with a specific energy of more than 380 Wh kg-1, counting all active and inactive components in a single cell, in particular with a high cathode loading, thin Li metal and lean electrolyte. The cycling life of the cell is increased by more than an order of magnitude compared to the cell using a flat Li-metal anode.

Niu, Chaojiang↗
DOE OSTI2020

A Numerical Study on the Impact of Cathode Catalyst Layer Loading on the Open Circuit Voltage

The open-circuit voltage (OCV) is the measured potential when no current is drawn from a cell. Additionally, theoretically this potential is given by the equilibrium potential, which is determined from thermodynamics based on the operating conditions. In practice, the actual potential at zero current is measured to be approximately 300 mV lower than the theoretical value.

42 ENGINEERING↗
DOE OSTI2018

A core–shell cathode substrate for developing high-loading, high-performance lithium–sulfur batteries

Lithium–sulfur batteries with a high theoretical energy density would be a promising next-generation energy-storage system if their cell-fabrication parameters (e.g., sulfur loading/content and the electrolyte/sulfur ratio) are improved to a practically necessary level. In this article, we report the design of a three-dimensional core–shell carbon substrate, integrating a porous internal core with a conductive external carbon nanofiber shell. Such a carbon substrate encapsulates a high amount of sulfur as the active material core to form a high-loading core–shell cathode, attaining an ultra-high sulfur loading and content of, respectively, 23 mg cm -2 and 75 wt%. With distinguishable internal and external regions, the carbon substrate facilitates the redox reactions and hinders the polysulfide diffusion. Therefore, the core–shell cathodes exhibit a high areal capacity and energy density of, respectively, 14 mA h cm -2 and 27 mW h cm -2 during cycling. During resting, they achieve a long shelf-life of one month with a low capacity-fade rate of 0.25% per day.

25 ENERGY STORAGE↗
DOE OSTI2018

TiS 2 –Polysulfide Hybrid Cathode with High Sulfur Loading and Low Electrolyte Consumption for Lithium–Sulfur Batteries

Sulfur cathodes have a high theoretical capacity of 1675 mAh g –1 , making the lithium–sulfur batteries a promising technology for future energy-storage devices. However, their commercial viability is faced with challenges arising from intrinsic electrochemical instabilities and inappropriate cell fabrication parameters. We report here the feasibility of employing TiS 2 as a conductive polysulfide adsorbent, which allows the use of a high amount of electrochemically active polysulfides in building a TiS 2 –polysulfide hybrid cathode. The hybrid cathode exhibits long cycle stability at a C/5 rate over 200 cycles with a high areal capacity and energy density of, respectively, 10 mAh cm –2 and 20 mWh cm –2 , exceeding those of commercial LiCoO 2 . Furthermore, such an enhanced electrochemical performance is obtained in cells with a high sulfur content (65 wt %), high sulfur loading (12 mg cm –2 ), high sulfur mass (12 mg/cathode), and a low electrolyte/sulfur ratio of just 5 μL mg –1 .

25 ENERGY STORAGE↗