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At least 667 records · Page 37
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Nanoporous Carbon Coatings Direct Li Electrodeposition Morphology and Performance in Li Metal Anode Batteries

Li metal anodes could significantly improve battery energy density. However, Li generally electrodeposits in poorly controlled morphology, leading to safety and performance problems. One factor that controls Li anode performance and electrodeposition morphology is the nature of the electrolyte–current collector interface. Herein, we modify the Cu current collector interface by depositing precisely controlled nanoporous carbon (NPC) coatings using pulsed laser deposition to develop an understanding of how NPC coating density and thickness impact Li electrodeposition. We find that NPC density and thickness guide Li morphological evolution differently and dictate whether Li deposits at the NPC-Cu or NPC-electrolyte interface. NPC coatings generally lower overpotential for Li electrodeposition, though thicker NPC coatings limit kinetics when cycling at a high rate. Lower-density NPC enables the highest Coulombic efficiency (CE) during calendar aging tests, and higher-density NPC enables the highest CE during cycling tests.

25 ENERGY STORAGE↗
DOE OSTI2020

Inhomogeneous distribution of lithium and electrolyte in aged Li-ion cylindrical cells

Carbonate-based electrolytes in Li-ion batteries exhibit long range order in a frozen state, which enables their non-destructive analysis by diffraction methods. In the current study the spatial distribution of lithium and electrolyte inside the graphite anode was determined in cycled Li-ion cells using monochromatic spatially-resolved neutron diffraction measurements at 150 K. The results indicate a loss of lithium and electrolyte and their non-uniform distribution in the graphite anode in aged Li-ion cells. The observed lithium and electrolyte losses are directly correlated with two electrochemical performance degradation mechanisms, which are responsible for the cell capacity fade.

18650-type↗
DOE OSTI2025

Modeling Electrodeposition in 3D Porous Architectures for Solid-State Li-Metal Batteries

Li-metal storage in three-dimensional (3D) electrodes is considered a potential dendrite-mitigation strategy. The large surface area and high porosity of these electrodes result in reduced local Li-plating current densities. The porous topology provides a scaffold for Li-deposition and stripping, maintaining both mechanical integrity and Li accessibility. The goal of this study is to understand how characteristics, such as geometry and material properties, affect the current distribution and deposition pattern. To this end, we developed a computational method to track material growth driven by electrodeposition within a complex geometry. This method ensures that the finite-element discretization remains conforming to the moving boundary while preserving an adequate mesh quality, and thus maintains solution accuracy. Using this new computational tool, we analyze the conditions under which porous anode architectures effectively expand the surface area of the charge-transfer interface, and self-regulate current density and dendrite growth.

3D electrode architectures↗
DOE OSTI2020

Investigating the Effects of Lithium Deposition on the Abuse Response of Lithium-Ion Batteries

Li deposition at the graphitic anode is widely reported in literature as one of the leading causes of capacity fade in lithium-ion batteries (LIBs). Previous literature has linked Li deposition resulting from low-temperature ageing to diminished safety characteristics, however no current research has probed the effects of Li deposition on the abuse response of well-characterized cells. Using overtemperature testing, a relationship between increased concentrations of Li deposition and exacerbated abuse response in 1 Ah pouch cells has been established. A novel Li deposition technique is also investigated, where cells with n:p < 1 (anode-limiting) have been cycled at a high rate to exploit Li + diffusion limitations at the anode. Scanning Electron Microscopy of harvested anodes indicates substantial Li deposition in low n:p cells after 20 cycles, with intricate networks of Li(s) deposits which hinder Li + intercalation/deintercalation. Peak broadening and decreased amplitude of differential capacity plots further validates a loss of lithium inventory to Li + dissolution, and Powder X-ray Diffraction indicates Li + intercalation with staging in anode interstitial sites as the extent of Li deposition increases. A cradle-to-grave approach is leveraged on cell fabrication and testing to eliminate uncertainty involving the effects of cell additives on Li deposition and other degradation mechanisms.

25 ENERGY STORAGE↗
DOE OSTI2023

Crystallographic Insight of Reduced Lattice Volume Expansion in Mesoporous Cu 2+ -Doped TiNb 2 O 7 Microspheres during Li + Insertion

TiNb 2 O 7 represents a promising anode material for lithium-ion batteries (LIBs), but its practical applications are currently hampered by the non-negligible volumetric expansion and contraction during the charge/discharge process and the sluggish ion/electron kinetics. Here a combination technique is reported by systematically optimizing the porous and spherical morphology, crystal structure, and surface decoration of mesoporous Cu 2+ -doped TiNb 2 O 7 microspheres to enhance the electrochemical Li + storage performance and stability simultaneously. The Cu 2+ dopants preferentially replace Ti 4+ in crystal lattices, which decreases the Li + diffusion barrier and increases the electronic conductivity, as confirmed by density functional theory (DFT) calculation and demonstrated by diverse electrochemical characterizations. The successful Cu 2+ doping significantly reduces the lattice expansion coefficient from 7.26% to 4.61% after Li + insertion along the b-axis of TiNb 2 O 7 , as visualized from in situ and ex situ XRD analysis. The optimal 5% Cu 2+ -doped TiNb 2 O 7 with surface coating of N-doped carbon exhibits significantly enhanced specific capacity and rate and cyclic performances in both half- and full-cell configurations, demonstrating an excellent electrochemical behavior for fast-charging LIB applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Benzene Ring Knitting Achieved by Ambient-Temperature Dehalogenation via Mechanochemical Ullmann-Type Reductive Coupling

The current approaches capable of affording conjugated porous networks (CPNs) still rely on solution-based coupling reactions promoted by noble metal complexes or Lewis acids, on-surface polymerization conducted in ultrahigh-vacuum environment at very high temperatures (>200 °C), or mechanochemical Scholl-type reactions limited to electron-rich substrates. To develop simple and scalable approaches capable of making CPNs under neat and ambient conditions, herein, a novel and complementary method to the current oxidative Scholl coupling processes is demonstrated to afford CPNs via direct aromatic ring knitting promoted by mechanochemical Ullmann-type reactions. The key to this strategy lies in the dehalogenation of aromatic halides in the presence of Mg involving the formation of Grignard reagent intermediates. Products (Ph-CPN-1) obtained via direct C-C bond formation between 1,2,4,5-tetrabromobenzene (TBB) monomer feature high surface areas together with mesoporous architecture. The versatility of this approach is confirmed by the successful construction of various CPNs via knitting of the corresponding aromatic rings (e.g., pyrene and triphenylene), and even highly crystalline graphite product was obtained. The CPNs exhibit good electrochemical performance as the anode material in lithium-ion batteries (LIBs). Overall, this approach expands the frontiers of CPN synthesis and provides new opportunities to their scalable applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multifunctional Coatings on Sulfide‐Based Solid Electrolyte Powders with Enhanced Processability, Stability, and Performance for Solid‐State Batteries

Abstract Sulfide‐based solid‐state electrolytes (SSEs) exhibit many tantalizing properties including high ionic conductivity and favorable mechanical properties for next‐generation solid‐state batteries. Widespread adoption of these materials is hindered by their intrinsic instability under ambient conditions, which makes them difficult to process at scale, and instability at the Li||SSE and cathode||SSE interfaces, which limits cell performance and lifetime. Atomic layer deposition is leveraged to grow thin Al 2 O 3 coatings on Li 6 PS 5 Cl powders to address both issues simultaneously. These coatings can be directly grown onto Li 6 PS 5 Cl particles with negligible chemical modification of the underlying material and enable exposure of powders to pure and H 2 O‐saturated oxygen environments for ≥4 h with minimal reactivity, compared with significant degradation of the uncoated powder. Pellets fabricated from coated powders exhibit ionic conductivities up to 2× higher than those made from uncoated material, with a simultaneous decrease in electronic conductivity and significant suppression of chemical reactivity at the Li‐SSE interface. These benefits result in significantly improved room temperature cycle life at high capacity and current density. It is hypothesized that this enhanced performance derives from improved intergranular properties and improved Li metal adhesion. This work points to a completely new framework for designing active, stable, and scalable materials for next‐generation solid‐state batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Highly Efficient Organosulfur and Lithium‐Metal Hosts Enabled by C@Fe 3 N Sponge

Abstract Lithium‐organosulfur (Li‐OS) batteries, despite possessing high theoretical specific capacity, encounter a few practical challenges, including unsatisfactory lifespan and low active material utilization under realistic conditions. Here, diisoropyl xanthogen polysulfide (DIXPS) has been selected as a model organosulfur compound to investigate the practical feasibility of Li‐OS batteries under realistic conditions. A well‐designed freestanding carbon sponge decorated with Fe 3 N nanoparticles (C@Fe 3 N) is introduced into the Li‐OS cells as a scaffold for both Li and DIXPS. The lithiophilic property of the C@Fe 3 N host guides uniform lithium deposition at the anode, and the catalysis of the DIXPS conversion reaction promotes the kinetics at the cathode. Impressively, the synergistic effect of C@Fe 3 N leads to an extremely stable cycling performance over 1 000 cycles in a Li‐OS full cell under realistic conditions.

He, Jiarui↗
DOE OSTI2025

Lithium‐Containing Hybrid SEI Layer Enabling High Mass Loading and Anode‐Less Sodium Metal Batteries

Abstract The continuous rupturing and rebuilding of unstable solid electrolyte interphase (SEI) layer during cycling would block Na + diffusion and induce Na dendrite formation, ultimately limiting the practical application of high‐energy‐density sodium metal batteries. Herein, a hybrid SEI layer containing Li‐species is dexterously constructed on the surface of sodium metal anode. Li‐containing inorganic components (Li 3 N, LiF, and Li 2 CO 3 ) are introduced to stabilize the Na/electrolyte interface and enhance the mechanical and diffusion kinetic properties of the SEI layer, which can reduce the side reactions and gas generation, regulate Na + flux during cycling and promote rapid Na + migration for uniform dendrite‐free Na deposition. As a result, the constructed Na symmetric cells achieve low overpotential and long cycle life of 5900, 1800, and 500 h at current densities of 3, 10, and 30 mA cm −2 , respectively. Furthermore, the full cells paired with the Na₃V₂(PO₄)₃ cathode demonstrate high specific capacity and excellent cycle stability, even at an ultra‐high cathode loading of 39.3 mg cm −2 and a low N/P ratio (negative/positive electrode capacity ratio of 1.21).

Xia, Li [State Key Laboratory of Physical Chemistr↗
DOE OSTI2022

Highly Efficient Organosulfur and Lithium-Metal Hosts Enabled by C@Fe 3 N Sponge

Lithium-organosulfur (Li-OS) batteries, despite possessing high theoretical specific capacity, encounter a few practical challenges, including unsatisfactory lifespan and low active material utilization under realistic conditions. Here, diisoropyl xanthogen polysulfide (DIXPS) has been selected as a model organosulfur compound to investigate the practical feasibility of Li-OS batteries under realistic conditions. A well-designed freestanding carbon sponge decorated with Fe 3 N nanoparticles (C@Fe 3 N) is introduced into the Li-OS cells as a scaffold for both Li and DIXPS. The lithiophilic property of the C@Fe 3 N host guides uniform lithium deposition at the anode, and the catalysis of the DIXPS conversion reaction promotes the kinetics at the cathode. Impressively, the synergistic effect of C@Fe 3 N leads to an extremely stable cycling performance over 1000 cycles in a Li-OS full cell under realistic conditions.

25 ENERGY STORAGE↗
DOE OSTI2025

Lithium‐Containing Hybrid SEI Layer Enabling High Mass Loading and Anode‐Less Sodium Metal Batteries

The continuous rupturing and rebuilding of unstable solid electrolyte interphase (SEI) layer during cycling would block Na + diffusion and induce Na dendrite formation, ultimately limiting the practical application of high-energy-density sodium metal batteries. Herein, a hybrid SEI layer containing Li-species is dexterously constructed on the surface of sodium metal anode. Li-containing inorganic components (Li 3 N, LiF, and Li 2 CO 3 ) are introduced to stabilize the Na/electrolyte interface and enhance the mechanical and diffusion kinetic properties of the SEI layer, which can reduce the side reactions and gas generation, regulate Na + flux during cycling and promote rapid Na + migration for uniform dendrite-free Na deposition. As a result, the constructed Na symmetric cells achieve low overpotential and long cycle life of 5900, 1800, and 500 h at current densities of 3, 10, and 30 mA cm −2 , respectively. Furthermore, the full cells paired with the Na₃V₂(PO₄)₃ cathode demonstrate high specific capacity and excellent cycle stability, even at an ultra-high cathode loading of 39.3 mg cm −2 and a low N/P ratio (negative/positive electrode capacity ratio of 1.21).

Diffusion kinetic↗
DOE OSTI2022

Lithium–Metal Batteries via Suppressing Li Dendrite Growth and Improving Coulombic Efficiency

Lithium–metal batteries (LMB) are recognized as one of the most promising candidates for the next generation of batteries due to their high energy density. Extensive studies have been refocused on the field in the past decade to make the technology commercially viable. Unfortunately, despite exciting progress that has been made, the practical application of LMBs is still hampered by the uncontrollable Li plating morphology and inferior Coulombic efficiency (CE) during cycling. Herein, first, the relevant research that has been carried out in the past decade (2010–2021) is briefly summarized and then the Li plating behaviors, mechanistic understanding of these behaviors, and strategies to suppress Li dendrite growth are discussed. Finally, the methods and techniques to improve Coulombic efficiency (CE) is discussed, especially the design of liquid electrolytes, and possible research directions for the future development of LMBs.

25 ENERGY STORAGE↗
DOE OSTI2023

Microstructure and defect engineering of graphite anodes by pulsed laser annealing for enhanced performance of lithium-ion batteries

We report nanosecond pulsed laser annealing significantly improves cyclability and current carrying capacity of lithium-ion batteries (LIBs). This improvement is achieved by engineering of microstructure and defect contents present in graphite in a controlled way by using pulsed laser annealing (PLA) to increase the number density of Li + ion trapping sites. The PLA treatment causes the following changes: (1) creates surface steps and grooves between the grains to improve Li + ion charging and intercalation rates; (2) removes inactive polyvinylidene difluoride (PVDF) binder from the top of graphite grains and between the grains which otherwise tends to block the Li + migration; and (3) produces carbon vacancies in (0001) planes which can provide Li + charging sites. From X-ray diffraction data, we find upshift in diffraction peak or reduction in planar spacing, from which vacancy concentration was estimated to be about 1.0%, which is higher than the thermodynamic equilibrium concentration of vacancies. The laser treatment creates single and multiple C vacancies which provide sites for Li + ions, and it also produces steps and grooves for Li + ions to enter the intercalating sites. It is envisaged that the formation of these sites enhances Li+ ion absorption during charge and discharge cycles. The current capacity increases from an average 360 mAh/g to 430 mAh/g, and C–V shows significant reduction in SEI layer formation after the laser treatment. If the vacancy concentration is too high and charge-discharge cycles are long, then trapping of electrons by Li + may occur, which can lead to Li 0 formation and Li plating causing reduction in current capacity.

25 ENERGY STORAGE↗
DOE OSTI2025

Unveiling the thermite-driven lithium fire ignition in solid-state batteries

Here, this study challenges the assumption of the non-flammability of lithium metal all-solid-state batteries (LiSSBs) and other lithium metal batteries without flammable electrolytes. Through thermodynamic calculations and ex situ experiments, we reveal for the first time the risk of thermite reactions between lithium metal and LiFePO 4 in both charged and discharged states. Reactivity is worsened by excess lithium metal in the cell, reaching final maximum adiabatic temperatures of 2,500°C in the charged state, which is hot enough to boil lithium. The thermite reaction triggers spontaneously at 500°C, with poor surface contact, while increasing surface contact through mixing initiates the reaction at room temperature in an inert environment. Despite its fast kinetics, this reaction is transport limited due to lithium passivation, leading to long burn times and reignition risks. Given the risk of lithium metal contacting the cathode during failure, understanding these reactions is crucial for ensuring the safe deployment of LiSSBs.

LiFePO4↗
DOE OSTI2025

Preparation and electrochemical properties of high-entropy oxide Li x (CrMnCoNiZn) 3-x O 4

High-entropy oxides (HEOs) have gained significant attention as anode materials for lithium-ion batteries (LIBs) due to their high theoretical specific capacity, synergistic effects of constituent elements, and enhanced structural stability induced by high entropy. Here, this study investigates the electrochemical properties of a novel series of HEOs, Li x (CrMnCoNiZn) 3-x O 4 , synthesized via the sol-gel method. As lithium content increases, the electrochemical lithium storage performance of the HEOs improves, attributed to the rise in high-valence states and oxygen vacancies. The high valence state of elements facilitates greater electron transfer, enhancing the specific capacity during lithium insertion. Additionally, a higher concentration of oxygen vacancies boosts ionic conductivity and lithium ion diffusion kinetics, leading to superior electrochemical performance. Among the synthesized materials, Li 0.11 (CrMnCoNiZn) 2.89 O 4 exhibited the best performance, delivering a discharge capacity of 365 mAh·g −1 after 100 cycles at 100 mA·g −1 , 257 mAh·g −1 after 1000 cycles at 1 A·g −1 , and a rate capacity of 196 mAh·g −1 at 2 A·g −1 . The Li + diffusion coefficient reached 2.78 × 10 −15 cm 2 ·s −1 . This work not only deepens the understanding of HEOs' electrochemical behavior in LIBs but also provides insights into the impact of lithium ion substitution on their performance.

25 ENERGY STORAGE↗
DOE OSTI2020

Sweeping potential regulated structural and chemical evolution of solid-electrolyte interphase on Cu and Li as revealed by cryo-TEM

A fundamental understanding of solid-electrolyte interphase (SEI) is paramount importance for controlling the cycling performance of rechargeable lithium metal batteries. The structural and chemical evolution of SEI with respect to electrochemical operating condition remains barely established. Here we develop a unique method for imaging the evolution of SEI formed on the Cu foil under sweeping electrochemical potential. By using cryogenic TEM imaging combined with energy dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy electronic structure analyses, we reveal that, for the vinylene carbonate (VC)-free electrolyte, the SEI formed at 1.0 V is a monolithic amorphous structure, which evolves to amorphous matrix embedded with Li 2 O particles as the voltage decreases to 0 V. In the case of VC-containing electrolyte, the SEI is featured by an amorphous matrix with Li 2 O particles from 1.0 V to 0 V. The thickness of SEI formed on Cu foil increases with decreasing voltage. Associated with the localized charge modulation by the surface topographic feature and defects in the Cu foil, the SEI layer shows direct spatial correlation with these structural defects in the Cu. In addition, upon Li deposition, the SEI formed on the Li metal has similar thickness with, but different composition from the SEI formed on the Cu foil at 0 V. Furthermore, those results provide insight toward SEI engineering for enhanced cycling stability of Li metal.

25 ENERGY STORAGE↗