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DOE OSTI2023

Understanding and controlling lithium morphology in solid polymer and gel polymer systems: mechanisms, strategies, and gaps

Lithium metal anode promises the highest theoretical energy density and may enable high energy designs such as lithium–sulfur and lithium–air batteries. However, stable lithium plating and stripping remains a challenge in all electrolyte systems including liquids, polymers, and ceramic electrolytes. In this perspective, we examine literature studies of lithium morphologies in solid polymer and gel polymer systems and compare that with well-studied liquid electrolytes. In solid polymer electrolytes, current density and mechanical properties are both governing parameters for lithium morphology, differing from conventional liquid electrolytes. Stable lithium electrodeposition may be accomplished by a polymer electrolyte with good stiffness operating at significantly lower current densities than its limiting current density, which is defined by the Sand equation. In gel polymer electrolytes, the reported lithium morphology is more similar to that in liquid electrolytes, suggesting similar nucleation and growth mechanisms. Based on experimental evidence and theoretical guidance, current strategies to control lithium morphology in solid polymer and gel polymer electrolytes are summarized. The limitations of these strategies are discussed. In particular, we note the knowledge gap in understanding the solid electrolyte interphase in solid polymer systems and the critical role it can play in regulating lithium morphologies.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Visualizing diverse lithium growth and stripping behaviors in anode-free solid-state batteries with operando X-ray tomography

Anode-free solid-state batteries (SSBs), which eliminate the need for lithium metal use during cell assembly, have the potential to enable high energy densities and simplified manufacturing. However, the factors that control lithium growth/stripping at the anode current collector are not well understood. Here, we use operando X-ray microcomputed tomography to comprehensively image and quantify lithium deposition and stripping under various conditions in three different Li|Li 6 PS 5 Cl|current collector cells, revealing diverse behavior that depends on interface morphology, cell resistance, and solid-state electrolyte (SSE) microstructure. A cell with high resistance exhibits extensive lithium filament growth across the entire current collector interface, with filaments that grow around pre-existing pores in the SSE rather than lithium filling these pores. Lithium filament formation is partially reversible, with the cracks shrinking as lithium metal is stripped. Uniform lithium deposition is achievable at low current densities in low-resistance cells, whereas higher current densities in these cells cause an increase in interfacial roughness, which is correlated with subsequent filamentary growth at the edges of the cell. These results provide insight into filamentary vs. planar lithium growth and highlight that the evolution of lithium is sensitively dependent on SSE microstructure and electrochemical processes.

25 ENERGY STORAGE↗

DOE OSTI2023

High capacity, air-stable, structurally isomorphous lithium alloy multilayer porous foams

The invention relates to composite multilayer lithium ion battery anodes that include a porous metal alloy foam, and a lithium ion conductor coating applied to the metal alloy foam. The metal alloy foam can include structurally isomorphous alloys of lithium and, optionally, lithium and magnesium. The lithium ion conductor coating can include ternary lithium silicate, such as, lithium orthosilicate. Lithium ions from the ternary lithium silicate may be deposited within the pores of the metal alloy foam. Optionally, the lithium ion conductor coating may include a dopant. The dopant can include one or more of magnesium, calcium, vanadium, niobium and fluorine, and mixtures and combinations thereof.

Kumta, Prashant N.↗

DOE OSTI2023

Probing the Effectiveness in Stabilizing Lithium Metal Anodes through Functional Additives

A variety of electrolyte additives were comprehensively evaluated to understand their relative capability in stabilizing lithium metal anode. Although the Li||Cu test is an effective test to rule out ineffective additives, a reliable assessment of individual additives cannot be obtained just by a single evaluation method. Therefore, various methods must be combined to truly assess the stabilization of a lithium anode. Moreover, it was also discovered that a significant depletion of electrolytes occurred during the end-of-life of the lithium batteries, which partially contributed to the sudden failure of the lithium batteries during cycling. However, the main culprit of the sudden failure was identified as the significant increase in the resistance of the lithium metal anode. Further, when used as an additive, cyclic fluorinated carbonates are the most effective in stabilizing the lithium anode and improving the cycling performance of lithium batteries among all the common additives. Despite its cost-effectiveness, the additive in the conventional electrolyte approach provides insufficient protection for lithium metal due to the complete consumption of the additive materials, which is necessary to repair the solid-electrolyte interphase (SEI). Therefore, it is suggested that a larger ratio (>15 wt %) of the SEI former should be employed to achieve effective lithium stabilization.

25 ENERGY STORAGE↗

DOE OSTI2021

Life Cycle Assessment and Techno-Economic Assessment of Lithium Recovery from Geothermal Brine

Lithium-ion batteries (LIB) play an essential role in the electrification of the transportation sector, and battery demand for lithium compounds will see a significant increase in the coming decades. This has raised concerns on the supply of lithium, and as a result, technologies are being developed to process unconventional lithium sources. One promising technology is to extract lithium from geothermal brine using lithium-aluminum-layered double hydroxide chloride (LDH) sorbent and forward osmosis. A combined life cycle assessment (LCA) and techno-economic assessment (TEA) is conducted to evaluate the environmental and economic performance of this technology. It is assumed that the lithium extraction unit is an add-on to a 50 MW geothermal power plant located in California. The analysis is based on lab-scale experimental data and stoichiometry while considering the economy of scale for an industrial system. LCA results suggest that, compared with conventional LiOH and Li 2 CO 3 production pathways, the new technology achieves 1–95% reduction in environmental impacts. Even higher reduction can be achieved for LiOH produced via electrolysis. This add-on unit for lithium extraction could achieve a payback period of less than 1 year and reach net present values of $454M and $315M and internal rates of return of 792 and 1130% for LiOH and Li 2 CO 3 production pathways, respectively. The favorable environmental and economic performance suggests that LDH sorption coupled with forward osmosis has great potential to enable the domestic production of battery lithium compounds and that further development should be carried out.

15 GEOTHERMAL ENERGY↗

DOE OSTI2021

Lithium superoxide encapsulated in a benzoquinone anion matrix

Lithium peroxide is the crucial storage material in lithium–air batteries. Understanding the redox properties of this salt is paramount toward improving the performance of this class of batteries. Lithium peroxide, upon exposure to p –benzoquinone (p–C 6 H 4 O 2 ) vapor, develops a deep blue color. This blue powder can be formally described as [Li 2 O 2 ] 0.3 • [LiO 2 ] 0.7 • {Li[p–C 6 H 4 O 2 ]} 0.7 , though spectroscopic characterization indicates a more nuanced structural speciation. Infrared, Raman, electron paramagnetic resonance, diffuse-reflectance ultraviolet-visible and X-ray absorption spectroscopy reveal that the lithium salt of the benzoquinone radical anion forms on the surface of the lithium peroxide, indicating the occurrence of electron and lithium ion transfer in the solid state. As a result, obligate lithium superoxide is formed and encapsulated in a shell of Li[p–C 6 H 4 O 2 ] with a core of Li 2 O 2 . Lithium superoxide has been proposed as a critical intermediate in the charge/discharge cycle of Li–air batteries, but has yet to be isolated, owing to instability. The results reported herein provide a snapshot of lithium peroxide/superoxide chemistry in the solid state with redox mediation.

25 ENERGY STORAGE↗

DOE OSTI2023

Incombustible Polymer Electrolyte Boosting Safety of Solid–State Lithium Batteries: A Review

Lithium-ion batteries with their portability, high energy density, and reusability are frequently used in today's world. Under extreme conditions, lithium-ion batteries leak, burn, and even explode. Therefore, improving the safety of lithium-ion batteries has become a focus of attention. Researchers believe using a solid electrolyte instead of a liquid one can solve the lithium battery safety issue. Due to the low price, good processability and high safety of the solid polymer electrolytes, increasing attention have been paid to them. However, polymer electrolytes can also decompose and burn under extreme conditions. Moreover, lithium dendrites are formed continuously due to the uneven charge distribution on the surface of the lithium metal anode. A short circuit caused by a lithium dendrite can cause the battery to thermal runaway. As a result, the safety of polymer solid-state batteries remains a challenge. In this review, the thermal runaway mechanism of the batteries is summarized, and the batteries abuse test standard is introduced. In addition, the recent works on the high-safety polymer electrolytes and the solution strategies of lithium anode problems in polymer batteries are reviewed. Finally, the development direction of safe polymer solid lithium batteries is prospected.

25 ENERGY STORAGE↗

DOE OSTI2022

Solvent-Free Manufacturing of Lithium-Ion Battery Electrodes via Cold Plasma

Slurry casting has been used to fabricate lithium-ion battery electrodes for decades, which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering. This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials, enabling solvent-free manufacturing electrodes with any electrochemistry of choice. The cold-plasma-coating technique enables fabricating electrodes with thickness (>200 μm), high mass loading (>30 mg cm -2 ), high peel strength, and the ability to print lithium-ion batteries in an arbitrary geometry. This crosscutting, chemistry agnostic, platform technology would increase energy density, eliminate the use of solvents, vacuum drying, and calendering processes during production, and reduce manufacturing cost for current and future cell designs. Here, lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique. It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes. Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6% over 500 cycles. For the highly conductive cathode material lithium cobalt oxide, an areal capacity of 4.2 mAh cm -2 at 0.2 C is attained. We anticipate that this new, highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.

25 ENERGY STORAGE↗

DOE OSTI2021

Uncovering the Relationship between Aging and Cycling on Lithium Metal Battery Self-Discharge

Lithium metal is considered the “holy grail” material to replace typical Li-ion anodes due to the absence of a host structure coupled with a high theoretical capacity. The absence of a host structure results in large volumetric changes when lithium is electrodeposited/dissolved, making the lithium prone to stranding and parasitic reactions with the electrolyte. Lithium research is focused on enabling highly reversible lithium electrodeposition/dissolution, which is important to achieving long cycle life. Understanding the various mechanisms of self-discharge is also critical for realizing practical lithium metal batteries but is often overlooked. In contrast to previous work, it is shown here that self-discharge via galvanic corrosion is negligible, particularly when lithium is cycled to relevant capacities. Rather, the continued electrochemical cycling of lithium metal results in self-discharge when periodic rest is applied during cycling. The extent of self-discharge can be controlled by increasing the capacity of plated lithium, tuning electrolyte chemistry, incorporating regular rest, or introducing lithiophilic materials. Finally, the Coulombic losses that occur during periodic rest are largely reversible, suggesting that the dominant self-discharge mechanism in this work is not an irreversible chemical process but rather a morphological process.

25 ENERGY STORAGE↗

DOE OSTI2025

Unveiling the Role of Lithium Iodide in Stabilizing Solid Interfaces in All-Solid-State Li Metal Batteries

A critical challenge in all-solid-state lithium metal batteries (ASSLMBs) is achieving a stable interface between the lithium metal anode and the solid electrolyte. Leveraging its success in Li/I 2 batteries, lithium iodide has garnered significant attentions for its potential to enhance interfacial stability and overall cell performance in ASSLMBs. Here, we elucidate the role of lithium iodide in stabilizing the solid interface in all-solid-state Li metal batteries with a Li argyrodite electrolyte, particularly focusing on its influence on lithium deposition behavior and interfacial evolution. Through in situ optical imaging, we demonstrate more uniform lithium deposition on an iodide-contained argyrodite electrolyte compared to a chloride-based counterpart. Complementary density functional theory calculations attribute improved lithium plating behavior to the enhanced lithiophilicity and better ionic conductivity of lithium iodide at the solid interface, effectively reducing localized current density. In conclusion, these findings provide useful insights into the mechanisms through which lithium iodide enhances the interfacial stability in ASSLMBs.

Anions↗

DOE OSTI2024

Evaluation of lithium as a tritium storage medium for betavoltaics

Lithium foils were demonstrated to absorb surrogate protium for tritium-powered betavoltaics. 20μm thick lithium foils were hole-punched from a ribbon of electrodeposited lithium on copper foil. The lithium foils were loaded with hydrogen in a custom Sievert apparatus where the pressure drop showed full hydriding at a hydrogen pressure of 2 bar and at all loading temperatures above the lithium melting point at 190, 200, 225, 250, and 300. Lithium hydride formation was confirmed with Raman spectroscopy after hydrogen loading. The kinetics of experimental hydride formation was compared to the diffusion-limited Mintz–Bloch model. While the Mintz–Bloch model showed good fit with the experimental loadings, the model overpredicted the loading kinetics starting at 250 °C and at higher temperatures. In conclusion, The overprediction was either caused by lithium hydride outgassing due to some reduction with some residual lithium hydroxide created from brief air exposure when sealing the lithium in the reactor or a transition from diffusion-limited hydride growth to surface or metal–hydride interface-limited hydride growth.

25 ENERGY STORAGE↗

DOE OSTI2021

Techno-Economic Analysis of Lithium Extraction from Geothermal Brines

The United States has a large, domestic source of lithium in geothermal fluids, especially at the Salton Sea region of southern California, where estimates of lithium pass-through at geothermal plants exceed 24,000 metric tons per year, based on 2019 geothermal plant operations. Lithium extraction from geothermal brines offers the potential to provide the United States with a secure, domestic supply of lithium to meet the increasing demands of electric vehicles, grid energy storage, portable electronics, and other end-use applications. Additionally, the use of direct extraction technologies allows for a more sustainable lithium supply relative to current evaporative brine and hardrock mining operations in terms of land use, water use, time to market with lithium products, and carbon intensity of operations. This report is part of an effort to assess geothermal brines as a source of commercial lithium supply for the United States. In this study, the National Renewable Energy Laboratory (NREL) reviews and summarizes public technoeconomic analyses of lithium extraction technologies. The work was coordinated with the Critical Minerals Institute at the Colorado School of Mines who focused on supply chain analysis of lithium.

15 GEOTHERMAL ENERGY↗

DOE OSTI2022

Mitigating Interfacial Mismatch between Lithium Metal and Garnet-Type Solid Electrolyte by Depositing Metal Nitride Lithiophilic Interlayer

Solid-state lithium batteries are generally considered as the next-generation battery technology that benefits from inherent nonflammable solid electrolytes and safe harnessing of high-capacity lithium metal. Among various solid-electrolyte candidates, cubic garnet-type Li 7 La 3 Zr 2 O 12 ceramics hold superiority due to their high ionic conductivity (10 –3 to 10 –4 S cm -1 ) and good chemical stability against lithium metal. However, practical deployment of solid-state batteries based on such garnet-type materials has been constrained by poor interfacing between lithium and garnet that displays high impedance and uneven current distribution. Herein, we propose a facile and effective strategy to significantly reduce this interfacial mismatch by modifying the surface of such garnet-type solid electrolyte with a thin layer of silicon nitride (Si 3 N 4 ). This interfacial layer ensures an intimate contact with lithium due to its lithiophilic nature and formation of an intermediate lithium–metal alloy. The interfacial resistance experiences an exponential drop from 1197 to 84.5 Ω cm 2 . Lithium symmetrical cells with Si 3 N 4 -modified garnet exhibited low overpotential and long-term stable plating/stripping cycles at room temperature compared to bare garnet. Furthermore, a hybrid solid-state battery with Si 3 N 4 -modified garnet sandwiched between lithium metal anode and LiFePO 4 cathode was demonstrated to operate with high cycling efficiency, excellent rate capability, and good electrochemical stability. This work represents a significant advancement toward use of garnet solid electrolytes in lithium metal batteries for the next-generation energy storage devices.

25 ENERGY STORAGE↗

DOE OSTI2019

An ultrathin ionomer interphase for high efficiency lithium anode in carbonate based electrolyte

High coulombic efficiency and dendrite suppression in carbonate electrolytes remain challenges to the development of high-energy lithium ion batteries containing lithium metal anodes. Here we demonstrate an ultrathin (≤100 nm) lithium-ion ionomer membrane consisting of lithium-exchanged sulfonated polyether ether ketone embedded with polyhedral oligosilsesquioxane as a coating layer on copper or lithium for achieving efficient and stable lithium plating-stripping cycles in a carbonate-based electrolyte. Operando analyses and theoretical simulation reveal the remarkable ability of the ionomer coating to enable electric field homogenization over a considerably large lithium-plating surface. The membrane coating, serving as an artificial solid-electrolyte interphase filter in minimizing parasitic reactions at the electrolyte-electrode interface, enables dendrite-free lithium plating on copper with outstanding coulombic efficiencies at room and elevated (50 °C) temperatures. The membrane coated copper demonstrates itself as a promising current collector for manufacturing high-quality pre-plated lithium thin-film anode.

25 ENERGY STORAGE↗

DOE OSTI2022

Electrical resistance of the current collector controls lithium morphology

Abstract The electrodeposition of low surface area lithium is critical to successful adoption of lithium metal batteries. Here, we discover the dependence of lithium metal morphology on electrical resistance of substrates, enabling us to design an alternative strategy for controlling lithium morphology and improving electrochemical performance. By modifying the current collector with atomic layer deposited conductive (ZnO, SnO 2 ) and resistive (Al 2 O 3 ) nanofilms, we show that conductive films promote the formation of high surface area lithium deposits, whereas highly resistive films promote the formation of lithium clusters of low surface area. We reveal an electrodeposition mechanism in which radial diffusion of electroactive species is promoted on resistive substrates, resulting in lateral growth of large (150 µm in diameter) planar lithium deposits. Using resistive substrates, similar lithium morphologies are formed in three distinct classes of electrolytes, resulting in up to ten-fold improvement in battery performance. Ultimately, we report anode-free pouch cells using the Al 2 O 3 -modified copper that maintain 60 % of their initial discharge capacity after 100 cycles, displaying the benefits of resistive substrates for controlling lithium electrodeposition.

25 ENERGY STORAGE↗

DOE OSTI2019

Model systems for screening and investigation of lithium metal electrode chemistry and dendrite formation

The use of lithium metal as an electrode for electrochemical energy storage will provide a significant impact on practical energy storage technology. Unfortunately, the use of lithium metal is plagued with challenging chemical problems. Specifically, the formation of a solid electrolyte interphase layer and the nucleation and growth of lithium dendrites: both must be addressed and controlled in order to achieve a practically useable pure lithium metal electrode. Currently sophisticated experimental techniques and computationally expensive simulations are being used to probe these problems but these methods are arduous and time consuming which delays timely evaluation and insight into the rapidly changing field of advanced energy storage. Here, we report the use of DFT simulations of lithium nanoclusters to investigate and explore lithium metal chemistry with inexpensive computational methods to gain greater insight into electrochemical reductions and the nucleation and growth of dendrites. DME, LiTFSI, and LiFSI reduction energetics and structures with electrode effects from lithium metal are reported providing better physical description of the absolute reduction potential characterization. The electronic structure of the lithium nanoclusters were used to investigate the nucleation and growth of lithium dendrites from an ab initio perspective. The results demonstrate that kinetic processes have more control over non uniform growth than thermodynamic processes. Based on this information, a non ab initio model was created in Matlab that shows the initial stages of dendrite nucleation considering approximately 2000 atoms.

25 ENERGY STORAGE↗

DOE OSTI2021

MoS 2 for beyond lithium-ion batteries

As a typical transition-metal chalcogenide material, molybdenum disulfide (MoS 2 ) has received tremendous attention because of its unique layered structure and versatile chemical, electronic, and optical properties. With the focus of this Perspective on the energy storage area, one of the most important contributions of MoS 2 is that it sparked the birth of the rechargeable lithium battery in the early 1980s, which later formed the foundation of commercial lithium batteries. After four decades, admitting that MoS 2 is still playing a significant role in the lithium-ion battery field and considerable effort was made to decipher the mechanism through ex situ and in situ studies and by means of MoS 2 nanostructure engineering that advances the lithium battery performance, it is also used in beyond lithium-ion batteries, such as sodium, magnesium, calcium, and aluminum energy storage systems. Such alternative battery systems are desirable because of the safety concerns of lithium and the depletion of lithium reserves and corresponding increase in cost. In this Perspective, recent development on the fabrication of novel MoS 2 nanostructures was discussed, followed by the scrutinization of their application in beyond lithium-ion batteries and the in situ/operando methods involved in these studies. Finally, a brief summary and outlook that may help with the future advancement of the beyond lithium-ion batteries are presented.

25 ENERGY STORAGE↗

DOE OSTI2024

Optimization of lithium vapor box divertor evaporator location on NSTX-U using SOLPS-ITER

Commercial fusion reactors will be faced with extremely high divertor target heat fluxes that will require mitigation. Simulations of detachment in an NSTX-U scenario projected to have 92 MW/m 2 unmitigated peak target heat flux are presented, which reaches sub-10 MW/m 2 target heat flux using a highly dissipating lithium vapor box divertor design. The lithium vapor box is a detached divertor design which employs lithium vapor evaporation and condensation to contain lithium below the X-point. Previous SOLPS modeling has indicated a lithium vapor box can reduce the heat flux down to 10 MW/m 2 via simultaneous evaporation from the Private Flux Region (PFR) and the Common Flux Region (CFR) sides of the vapor box. It is found here that PFR evaporation has improved access to the separatrix leading to significantly more efficient power dissipation than CFR evaporation. Simulations of target evaporation with an evaporation distribution that is self-consistent with the temperature of a Capillary Porous System with Fast flowing liquid lithium (CPSF) could reach n Li / n e ~ 0.025-0.030 at the Last Closed Flux Surface (LCFS) depending on the liquid metal flow speeds and lithium sputtering yield, while PFR-side evaporation can reach acceptable heat fluxes with n Li / n e ~ 0.038 at the LCFS. However, PFR evaporator performance can be improved if the target is allowed to be hot enough such that it reflects lithium, reaching n Li / n e ~ 0.028 and reducing required lithium evaporation. Ultimately PFR evaporation and target evaporation are found to have similar ability to produce acceptable heat flux solutions with minimal upstream concentration.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗