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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

The Impact of Lithium Anode Interface on Capacity Fade in Polymer Electrolyte-Based Solid-State Batteries

This study investigates the Li stripping-plating morphology and failure mechanisms in full cells consisting of a solid polymer electrolyte (SPE) with two commercial Li anodes: Li chip and Li foil. The primary identified failure mechanism of the SPE cell is capacity fade, regardless of the Li manufacturer. While the cathode’s role in capacity fade is evident, the Li anode significantly influences cycling performance, with Li foil cells cycling 50% longer than Li chip cells, a statistical difference. Further, post-mortem scanning electron microscopy and X-ray photoelectron spectroscopy results attribute the Li chip’s faster capacity fade to a loss of contact and continuous growth of the solid electrolyte interphase (SEI). Conversely, Li foil maintains consistent contact with the solid polymer, displaying a thin and stable SEI. Additionally, failure mechanisms between a gel electrolyte in previous work and the dry SPE are compared.

25 ENERGY STORAGE↗
DOE OSTI2025

A Universal Design of Lithium Anode via Dynamic Stability Strategy for Practical All‐Solid‐State Batteries

Abstract All‐solid‐state Li‐metal battery (ASSLB) chemistry with thin solid‐state electrolyte (SSE) membranes features high energy density and intrinsic safety but suffers from severe dendrite formation and poor interface contact during cycling, which hampers the practical application of rechargeable ASSLB. Here, we propose a universal design of thin Li‐metal anode (LMA) via a dynamic stability strategy to address these issues. The ultra‐thin LMA (20 μm) is in situ constructed with uniform highly Li‐ion conductive solid‐electrolyte interphase and composite‐polymer interphase (CPI) via electroplating process. As a result, the passivation layer with poor Li‐ion conduction on Li anode can be dissolved and small surface resistance can be achieved due to the good compatibility of CPI to SSEs. The cycling of Li symmetric cell with Li 6 PS 5 Cl thin film electrolyte (<100 μm) shows a high critical current density of >2.0 mA cm −2 with excellent cycling stability at 1.0 mA cm −2 . The ASSLBs paring with Ni‐rich LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode demonstrated the feasibility of engineered LMA design by presenting good rate capability from 0.1 C to 1.0 C at room temperature, as well as long‐term cycling stability (81 % retention after 100 cycles). This work represents a general pathway to make thin dendrite‐free LMA available for high‐energy‐density ASSLBs.

Deng, Tao [Department of Chemical and Biomolecular↗
DOE OSTI2025

A Universal Design of Lithium Anode via Dynamic Stability Strategy for Practical All‐Solid‐State Batteries

Abstract All‐solid‐state Li‐metal battery (ASSLB) chemistry with thin solid‐state electrolyte (SSE) membranes features high energy density and intrinsic safety but suffers from severe dendrite formation and poor interface contact during cycling, which hampers the practical application of rechargeable ASSLB. Here, we propose a universal design of thin Li‐metal anode (LMA) via a dynamic stability strategy to address these issues. The ultra‐thin LMA (20 μm) is in situ constructed with uniform highly Li‐ion conductive solid‐electrolyte interphase and composite‐polymer interphase (CPI) via electroplating process. As a result, the passivation layer with poor Li‐ion conduction on Li anode can be dissolved and small surface resistance can be achieved due to the good compatibility of CPI to SSEs. The cycling of Li symmetric cell with Li 6 PS 5 Cl thin film electrolyte (<100 μm) shows a high critical current density of >2.0 mA cm −2 with excellent cycling stability at 1.0 mA cm −2 . The ASSLBs paring with Ni‐rich LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode demonstrated the feasibility of engineered LMA design by presenting good rate capability from 0.1 C to 1.0 C at room temperature, as well as long‐term cycling stability (81 % retention after 100 cycles). This work represents a general pathway to make thin dendrite‐free LMA available for high‐energy‐density ASSLBs.

Deng, Tao [Department of Chemical and Biomolecular↗
DOE OSTI2023

Protective coatings for lithium anodes

A hybrid protective coating includes an inorganic component and an organic component such that the inorganic component includes at least one of a metal oxide, a metal fluoride, or combination thereof, and the organic component includes at least one metalcone.

Elam, Jeffrey W.↗
DOE OSTI2022

Understanding Solid-Electrolyte Interphase Formation at the Lithium Metal Anode of Lithium-Sulfur Batteries

Lithium-sulfur (Li-S) batteries are one of the most promising chemistries for the next generation of energy storage devices. In a standard Li-S cell, the metallic lithium anode is an essential component of the battery due to its low density, extremely high theoretical specific capacity, and very low negative electrochemical potential. However, several challenges related to the use of Li metal have prevented this battery technology from becoming commercially available. For instance, Li-anodes are highly reactive, which results in the continuous decomposition of the electrolyte and the formation of the solid-electrolyte interphase (SEI) layer. This, combined with the non-uniform deposition of Liions during plating at the anode surface, can seriously affect the performance, cycling, and safety of the battery. In addition, it has been suggested that a controlled SEI formation at the metallic Li anode can yield enhanced battery performance. Hence, a comprehensive understanding of how the SEI layer is formed can help elucidate improvements in this battery technology. In this work, the formation of the SEI layer in Li-S batteries is investigated using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. The stability of liquid organic-based electrolyte components, salt concentration, electron-rich environments, and the use of inorganic solid-state electrolyte (SSE) materials are explored in order to provide molecular-level fundamental insights into how the nature and composition of the electrolyte can alter the initial stages of the SEI formation. The products of electrolyte decomposition and electro-/chemical reaction pathways of liquid electrolyte component such as solvent and salts are predicted from AIMD simulations of electrolyte-anode interfaces. Energetics of reactions from DFT ground-state optimizations are also presented to confirm the decomposition mechanisms. Some significant differences are then drawn regarding the use of low and high salt concentrations. Simulations under electron-rich environments show additional multielectron electrochemical reactions of solvent and salt decomposition taking place due to the excess of electrons and the presence of radical anions in the solution. Finally, the initial stages of formation, stability, and main constituents of interfaces between Li-metal and Sbased electrodes with sulfide-based SSEs are characterized in detail.

25 ENERGY STORAGE↗
DOE OSTI2022

High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

Anode-free lithium–metal batteries (LMBs) are ideal candidates for high-capacity energy storage as they eliminate the need for a conventional graphite electrode or excess lithium–metal anode. Current anode-free LMBs suffer from low Coulombic efficiency (CE) due to poor lithium stripping efficiency. Advanced electrolyte development is a promising route to maximize lithium plating and stripping CE and minimize capacity fade. However, a poor understanding of the mechanisms by which advanced electrolytes improve performance hampers progress in the practical development of anode-free LMBs. Here, we use synchrotron techniques and other tools to analyze the influence of three commercially available electrolytes on the composition, heterogeneity, kinetics, morphology, and electrochemistry of anode-free LMBs. Advanced electrolytes improve the electrochemical performance of anode-free LMBs by forming much denser and better-packed Li morphologies on a Cu current collector than on the conventional electrolyte. Li plates uniformly over the electrode area with the advanced electrolytes rather than in a few active sites. Inactive crystalline Li with heterogeneous distribution dominates the capacity degradation of anode-free cells, especially with the conventional electrolyte, indicating that reducing the amount of “dead” crystalline Li will significantly improve the cycling stability of anode-free cells. Finally, the understanding of the Li plating and stripping process obtained from this work will accelerate the development of anode-free LMBs with high efficiency.

25 ENERGY STORAGE↗
DOE OSTI2022

Covalent Organic Framework as an Efficient Protection Layer for a Stable Lithium‐Metal Anode

Abstract Lithium (Li) metal shows great potential for achieving high‐energy‐density rechargeable batteries. However, the practical applications of Li‐metal batteries are still challenged by the formation of Li dendrites and unstable solid‐electrolyte interphase (SEI) on metallic Li. Herein, a thin covalent organic framework layer is in situ fabricated on Li (COF‐Li) to suppress Li dendrite growth and mitigate the side reaction on the Li anode. The COF has a periodic and uniform porosity, allowing for selectively sieving Li ions and guiding a uniform Li deposition. As a result, the COF‐Li exhibits a non‐dendrite morphology during repeated Li plating/stripping and demonstrates a remarkable cycle life over 13 200 h with an extremely low overpotential of only 16 mV at a high current density of 10 mA cm −2 and a high areal capacity of 10 mAh cm −2 .

He, Jiarui↗
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 OSTI2021

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

Abstract 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. Herein, 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.

Gao, Peiyuan↗
NASA NTRS1994

Development of Carbon Anode for Rechargeable Lithium Cells

Conventionally, rechargeable lithium cells employ a pure lithium anode. To overcome problems associated with the pure lithium electrode, it has been proposed to replace the conventional electrode with an alternative material having a greater stability with respect to the cell electrolytes. For this reason, several graphitic and coke based carbonaceous materials were evaluated as candidate anode materials...In this paper, we summarize the results of the studies on Li-ion cell development.

rechargeable batteries batteries lithium cells lit↗
DOE OSTI2022

Anode‐Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

Abstract The two major barriers of practical lithium–sulfur batteries are the poor reversibility of lithium‐metal anode and sluggish kinetics of sulfur cathode. Here, we report a simple yet cogent, molecular tailoring approach for lithium polysulfides, enabling a synergistic enhancement of anode reversibility and cathode kinetics. We show that SnI 4 coordinates with lithium polysulfides to form soluble complexes, resulting in a Li 2 SnS 3 ‐rich anode interphase layer. As Li 2 SnS 3 is stable against parasitic reactions and has a lower ionic resistance over cycling, the Li plating/stripping efficiency is greatly improved. In addition, the formation of soluble complexes between SnI 4 and lithium polysulfides play a non‐negligible role in suppressing the clustering behavior of lithium polysulfide molecules, resulting in a significant enhancement in sulfur conversion kinetics under lean electrolyte conditions. The synergistic improvement is validated in anode‐free, lean‐electrolyte pouch cells with a Li 2 S cathode that displays capacity retention of 78 % after 100 cycles.

Ren, Yuxun↗
DOE OSTI2022

Anode-Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

The two major barriers of practical lithium–sulfur batteries are the poor reversibility of lithium-metal anode and sluggish kinetics of sulfur cathode. Here, we report a simple yet cogent, molecular tailoring approach for lithium polysulfides, enabling a synergistic enhancement of anode reversibility and cathode kinetics. In this study, we show that SnI 4 coordinates with lithium polysulfides to form soluble complexes, resulting in a Li 2 SnS 3 -rich anode interphase layer. As Li 2 SnS 3 is stable against parasitic reactions and has a lower ionic resistance over cycling, the Li plating/stripping efficiency is greatly improved. In addition, the formation of soluble complexes between SnI 4 and lithium polysulfides play a non-negligible role in suppressing the clustering behavior of lithium polysulfide molecules, resulting in a significant enhancement in sulfur conversion kinetics under lean electrolyte conditions. The synergistic improvement is validated in anode-free, lean-electrolyte pouch cells with a Li 2 S cathode that displays capacity retention of 78 % after 100 cycles.

25 ENERGY STORAGE↗
DOE OSTI2022

Covalent Organic Framework as an Efficient Protection Layer for a Stable Lithium-Metal Anode

We report Lithium (Li) metal shows great potential for achieving high-energy-density rechargeable batteries. However, the practical applications of Li-metal batteries are still challenged by the formation of Li dendrites and unstable solid-electrolyte interphase (SEI) on metallic Li. Herein, a thin covalent organic framework layer is in situ fabricated on Li (COF-Li) to suppress Li dendrite growth and mitigate the side reaction on the Li anode. The COF has a periodic and uniform porosity, allowing for selectively sieving Li ions and guiding a uniform Li deposition. As a result, the COF-Li exhibits a non-dendrite morphology during repeated Li plating/stripping and demonstrates a remarkable cycle life over 13 200 h with an extremely low overpotential of only 16 mV at a high current density of 10 mA cm -2 and a high areal capacity of 10 mAh cm -2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

A Facile Potential Hold Method for Fostering an Inorganic Solid‐Electrolyte Interphase for Anode‐Free Lithium‐Metal Batteries

Abstract Anode‐free lithium batteries are regarded as an ultimate form of high‐energy‐density lithium‐ion batteries. Unfortunately, irreversible lithium loss during cycling plays a major role in degrading the overall cell performance in the anode‐free configuration. To alleviate the deterioration, building a robust solid‐electrolyte interface on an anode current collector is an indispensable requirement. Here, we present a facile in‐situ electrochemical method of a potential hold during the first charge to guide more salt‐derived (less solvent‐derived) decomposition on the anode interface. We show the distinctive decomposition potential of lithium salts and ether/carbonate solvents, where the Li‐solvation structures with salt contact‐ion‐pairs preferentially decompose to form LiF‐rich and less organic components, leading to enhanced lithium Coulombic efficiency in Li||Cu cells as well as mitigating the capacity fade of Cu||LiFePO 4 and Cu||LiNi 0.8 Mn 0.1 Co 0.1 O 2 cells.

Shin, Woochul↗
DOE OSTI2022

SEI formation mechanisms and Li + dissolution in lithium metal anodes: Impact of the electrolyte composition and the electrolyte-to-anode ratio

The lithium metal battery is one of today's most promising high-energy-density storage devices. Its full-scale implementation depends on solving operational and safety issues intrinsic to the Li metal high reactivity leading to uncontrolled electrolyte decomposition and uneven Li deposition. In this work, we study the spontaneous formation of the solid electrolyte interphase (SEI) upon contact of Li metal with the electrolyte and describe the heterogeneous SEI morphological features. Multiple electrolyte formulations based on lithium bis(fluorosulfonyl)imide (LiFSI), dimethoxyethane (DME), dimethyl carbonate (DMC), 1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) and bis(2,2,2-trifluoroethyl) ether (BTFE) are used. Findings include the description of the SEI evolution from dispersed LiO, LiS, LiN, and LiF clusters to a continuous and compact inorganic phase in which the LiO and LiF content depend on the presence of fluorine diluents. Further, the role of the DME ether solvent helping the growth of a “wet-SEI” is compared to that of the highly unstable carbonate DMC, which decomposes into complex radical oligomers that might contribute to further electrolyte decomposition. The impact of the electrolyte-to-anode ratio on LiFSI decomposition is highlighted. Finally, we suggest the existence of a critical LiFSI concentration and electrolyte-to-anode ratio that could potentially balance the rate of electrolyte depletion and lithium consumption.

25 ENERGY STORAGE↗