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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Kinetics Tuning the Electrochemistry of Lithium Dendrites Formation in Lithium Batteries through Electrolytes

Lithium batteries are one of the most advance energy storage devices in the world and have attracted extensive research interests. However, lithium dendrite growth was a safety issue which handicapped the application of pure lithium metal in the negative electrode. In this paper, two solvents, propylene carbonate (PC) and 2-methyl-tetrahydrofuran (2MeTHF), and four Li + salts, LiPF 6 , LiAsF 6 , LiBF 4 and LiClO 4 were investigated in terms of their effects on the kinetics of lithium dendrite formation in eight electrolyte solutions. The kinetic parameters of charge transfer step (exchange current density, j 0 , transfer coefficient, α) of Li + /Li redox system, the mass transfer parameters of Li + (transfer number of Li + , t Li+ , diffusion coefficient of Li + , D Li+ ), and the conductivity (κ) of each electrolyte were studied separately. The results demonstrate that the solvents play a critical role in the measured j 0 , t Li+ , D Li+ , and κ of the electrolyte, while the choice of Li + salts only slightly affect the measured parameters. Finally, the understanding of the kinetics will gain insight into the mechanism of lithium dendrite formation and provide guidelines to the future application of lithium metal.

2-methyl-tetrahydrofuran↗
DOE OSTI2019

Prospect of Thermal Shock Induced Healing of Lithium Dendrite

Dendritic growth plagues the development of rechargeable lithium metal anodes. Recently, it has been reported that self-heating of the cell provides a mitigation strategy for suppressing dendrites. In order to study this phenomenon, we extend our recently developed nonlinear phase-field model to incorporate an energy balance equation allowing a full thermally coupled electrodeposition model using the open-source software package MOOSE. In this study, we consider the interplay between ionic transport and electrochemical reaction rate as a function of temperature and explore the possibility of using thermal shock induced dendrite suppression. We discover that, depending on the electrochemical reaction barrier and ionic diffusion barrier, self-heating could accelerate (larger reaction barrier) or decelerate (larger diffusion barrier) dendrite formation. Given that the electrolyte constituents can be used to tune both barriers, this study could provide an important avenue to exploit the self-heating effect favorably through electrolyte engineering.

25 ENERGY STORAGE↗
DOE OSTI2019

Magnetic Field-Suppressed Lithium Dendrite Growth for Stable Lithium-Metal Batteries

Lithium metal is the most attractive anode material due to its extremely high specific capacity, minimum potential, and low density. However, uncontrollable growth of lithium dendrite results in severe safety and cycling stability concerns, which hinders the application in next generation secondary batteries. In this paper, a new and facile method imposing a magnetic field to lithium metal anodes is proposed. That is, the lithium ions suffering Lorentz force due to the electromagnetic fields are put into spiral motion causing magnetohydrodynamics (MHD) effect. This MHD effect can effectively promote mass transfer and uniform distribution of lithium ions to suppress the dendrite growth as well as obtain uniform and compact lithium deposition. The results show that the lithium metal electrodes within the magnetic field exhibit excellent cycling and rate performance in a symmetrical battery. Additionally, full batteries using limited lithium metal as anodes and commercial LiFePO 4 as cathodes show improved performance within the magnetic field. In summary, a new and facile strategy of suppressing lithium dendrites using the MHD effect by imposing a magnetic field is proposed, which may be generalized to other advanced alkali metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Unveiling the mechanisms of lithium dendrite suppression by cationic polymer film induced solid–electrolyte interphase modification

It is crucial to suppress lithium dendrite formation in lithium metal batteries. Formation of a good solid–electrolyte interphase (SEI) has been considered to be effective in limiting lithium dendrite growth. However, how the SEI may be modified during lithium deposition is hard to resolve due to challenges in in situ investigation of the SEI with fine details. Here, we report an in situ study that uncovers the lithium dendrite suppression mechanism arising from SEI modification by a poly(diallyldimethylammonium chloride) (PDDA) cationic polymer film, using electrochemical liquid cell transmission electron microscopy (TEM). Lithium nanogranules are obtained in the presence of the polymer film. Chemical mapping of the deposits provides remarkable details of the SEI on individual nanogranules. It shows that lithium fluorides are uniformly distributed within the inner SEI layer of individual lithium nanogranules, arising from the instantaneous reaction of the deposited lithium with PF 6 – ions accumulated by the cationic polymer film, and thus the dendritic growth of lithium is prohibited. The ability to directly measure SEI chemistry at the nanoscale down to the individual nanograins in situ and unveil its correlation with the lithium deposition behavior opens future opportunities to explore unsolved mechanisms in batteries.

25 ENERGY STORAGE↗
DOE OSTI2026

Self-Healing Lithium Dendrites through Spontaneous Passivating Layer Formation for Stable Solid-State Lithium–Metal Batteries

All-solid-state lithium–metal batteries have attracted significant attention, owing to their high energy density and superior safety. However, lithium–metal penetration through the solid electrolyte, leading to short-circuiting, remains a critical failure mode that demands comprehensive mitigation strategies. Most existing strategies are effective only prior to the initiation of lithium-dendrite formation and fail once dendrites begin to propagate through the electrolyte. In this study, we propose a self-healing mechanism in which the penetrated lithium reacts with a self-healing agent to form a passivating layer along the particle boundaries. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated into a Li 6 PS 5 Cl solid electrolyte as the self-healing agent to suppress lithium-dendrite propagation even after dendrite formation initiated under high current densities. The self-healing induced by LiTFSI was verified through comprehensive experimental analyses and was further demonstrated in a full-cell configuration. Moreover, LiTFSI incorporation plays an important role in increasing the critical current density by reducing the overall electronic conductivity of the solid electrolyte and facilitating the formation of a robust LiF-containing solid-electrolyte interphase.

25 ENERGY STORAGE↗
DOE OSTI2015

Lithium Dendrite Formation

Scientists at the Department of Energy’s Oak Ridge National Laboratory have captured the first real-time nanoscale images of lithium dendrite structures known to degrade lithium-ion batteries. The ORNL team’s electron microscopy could help researchers address long-standing issues related to battery performance and safety. Video shows annular dark-field scanning transmission electron microscopy imaging (ADF STEM) of lithium dendrite nucleation and growth from a glassy carbon working electrode and within a 1.2M LiPF6 EC:DM battery electrolyte.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Extending the Life of Lithium-Based Rechargeable Batteries by Reaction of Lithium Dendrites with a Novel Silica Nanoparticle Sandwiched Separator

A reaction-protective separator that slows the growth of lithium dendrites penetrating into the separator is produced by sandwiching silica nanoparticles between two polymer separators. Here, the reaction between lithium dendrites and silica nanoparticles consumes the dendrites and can extend the life of the battery by approximately five times.

25 ENERGY STORAGE↗
DOE OSTI2017

Direct Observation of the Growth of Lithium Dendrites on Graphite Anodes by Operando EC‐AFM

Abstract Lithium dendrite growth is one of the most challenging problems affecting the safety performance of lithium‐ion batteries (LIBs). It causes low Coulombic efficiency as well as safety hazards for LIBs. Understanding the evolution process of Li‐dendrite growth at the nanoscale is critical for solving this problem. Herein, an in situ electrochemical atomic force microscopy (EC‐AFM) investigation of the initial Li deposition in ethylene carbonate (EC)‐based and fluoroethylene carbonate (FEC)‐based electrolytes on graphite anodes is reported. These results show that the solid electrolyte interphase (SEI) formed from the FEC‐based electrolyte can suppress Li‐dendrite growth. The FEC‐based electrolyte induces formation of LiF‐rich SEI films, which are harder and denser than those formed in an EC‐based electrolyte. Due to its better mechanical properties and larger resistance, the SEI layer formed from the FEC‐based electrolyte is sufficient to prevent reduction of Li + ions and deposition of Li + ions on the anode surface. These results demonstrate that EC‐AFM is a powerful in situ technique for the study of lithium‐dendrite growth.

Shen, Cai↗
DOE OSTI2018

CoO nanofiber decorated nickel foams as lithium dendrite suppressing host skeletons for high energy lithium metal batteries

Lithium metal is considered to be the most promising anode for the next-generation lithium batteries. However, dendrite growth due to uneven Li plating during battery cycling leads to short circuit and safety hazards, as well as shorted cycling life for the battery, which is the vital obstacle for the practical application of Li metal anode in lithium batteries. We report a CoO nanofiber decorated Ni foam (CONF) skeleton used as a 3D conductive host to suppress the dendrite formation for composite Li anode (CONF-Li) fabricated by thermal infusion method. The uniformly distributed CoO nanofibers on the Ni foam can improve the lithiophilicity of Ni foam, and decrease the local current inhomogeneity of the anode, leading to a mild and uniform Li plating/stripping behavior which effectively suppresses the Li dendrite formation. As a result, the electrochemical performances of CONF-Li anode are significantly improved both in symmetric cells and full cells (lithium-sulfur and lithium-LiNi 0.8 Co 0.15 Al 0.05 O 2 cells) proving its advancement over the pure Li anode.

25 ENERGY STORAGE↗
DOE OSTI2020

Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries

Abstract Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium–sulfur (Li‐S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li‐S pouch cells. Herein, we demonstrate that a rational combination of selenium doping, core–shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm −2 ) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm −2 ) with a low electrolyte/sulfur ratio (10 μL mg −1 ). This research further demonstrates a durable Li‐Se/S pouch cell with high specific capacity, validating the potential practical applications.

Zhao, Chen↗
DOE OSTI2018

Impact of External Pressure and Electrolyte Transport Properties on Lithium Dendrite Growth

Practical implementation of metal anodes in commercial lithium-ion batteries has been limited by the growth of dendritic protrusions, which can cause short-circuits and adversely affect battery safety. The impacts of the physical (such as external pressure and electrolyte shear modulus) and electrochemical (for example, conductivity, diffusivity and transference number) properties of a solid electrolyte on the propensity of lithium dendrite growth are investigated here. It is found that over a range of conditions, there are critical pressures above which growth of lithium dendritic protrusions can be prevented. The magnitude of this critical pressure depends on the elastic modulus of the electrolyte. Plastic deformation of lithium at high pressure results in reduced protrusion growth, which helps in obtaining stable deposition. For the first time, phase maps have been developed based on mechanical and transport properties of electrolytes, indicating conditions under which stable deposition of lithium is possible during long-term operation. Suppression of dendrites by individually altering conductivity, or diffusivity, or transference number, or elastic modulus of the electrolyte appears to be a relatively difficult task. Finally, minor tailoring of the transference number and elastic modulus of present-day polymer electrolytes, in a combined fashion, can lead to dendrite-free deposition of lithium.

25 ENERGY STORAGE↗
DOE OSTI2020

Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries

Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium-sulfur (Li-S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li-S pouch cells. In this work, we demonstrate that a rational combination of selenium doping, core-shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm -2 ) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm -2 ) with a low electrolyte/sulfur ratio (10 mu L mg(-1)). Overall, this research further demonstrates a durable Li-Se/S pouch cell with high specific capacity, validating the potential practical applications.

25 ENERGY STORAGE↗
DOE OSTI2018

Growth of Lithium Dendrites and Globules through a Solid Block Copolymer Electrolyte as a Function of Current Density

The uncontrollable nonplanar electrodeposition of lithium is a significant barrier to the widespread adoption of high energy density rechargeable batteries with a lithium metal anode. A promising approach for preventing the growth of lithium dendrites is the use of solid polymer electrolytes with a high shear modulus. Current density is the key variable in the electrodeposition of lithium. The present study is the first attempt at quantifying the effect of current density on the geometry and density of dendrites and other protrusions during electrodeposition through a solid polymer electrolyte. The geometry and density of defects formed on the lithium electrode were determined by X-ray microtomography. The tomograms revealed protrusions on the electrodeposited lithium electrodes that were either globular or dendritic, or void defects. The range of current densities over which stable, planar deposition was observed is quantified. At higher current densities, globular protrusions were observed. At the highest current density, both globular and dendritic protrusions were observed. The areal density of protrusion defects increased sharply with current density, while the overall defect density is a weak function of current density. Finally, our work enables comparisons between the experimentally determined onset of nonplanar electrodeposition and prevailing theoretical predictions with no adjustable parameters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Regulated lithium ionic flux through well-aligned channels for lithium dendrite inhibition in solid-state batteries

The utilization of solid electrolyte (SE) to suppress lithium (Li) dendrites is promising but still far from satisfactory due to the inhomogeneous Li plating/stripping. In this paper, we demonstrated a novel strategy to inhibit Li dendrites via regulating Li-ion flux in SE by using vertically aligned channels. The ion-insulating walls facilitated uniform distribution of Li-ion flux through the channels, leading to a homogeneous Li deposition, thus alleviating Li dendrite formation. As a result, symmetric cells with this SE exhibited excellent long-term stability (1000 h) against Li metal. In addition, Li4Ti5O12 (LTO)/Li cell with the developed SE achieved good battery performance over 100 cycles. The mechanism for dendrite suppression was further investigated by phase-field simulation. This work provides a novel strategy by manipulating uniform Li-ion flux to fabricate SE to inhibit Li dendrites and facilitates the development of high-performance rechargeable Li batteries.

25 ENERGY STORAGE↗