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Search Results (914)

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Keywords = lithium metal battery

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5 pages, 142 KiB  
Editorial
Manufacturing and Characterization of Metallic Electrode Materials
by Que Huang
Metals 2025, 15(8), 882; https://doi.org/10.3390/met15080882 - 7 Aug 2025
Abstract
In recent years, the growing demand for resources has driven the development of energy storage devices and related technologies, particularly the application of metal electrode materials, which are of particular importance in lithium, sodium, potassium, and zinc-based ion batteries, metal batteries, and solar [...] Read more.
In recent years, the growing demand for resources has driven the development of energy storage devices and related technologies, particularly the application of metal electrode materials, which are of particular importance in lithium, sodium, potassium, and zinc-based ion batteries, metal batteries, and solar energy storage and catalytic technologies [...] Full article
(This article belongs to the Special Issue Manufacturing and Characterization of Metallic Electrode Materials)
32 pages, 8366 KiB  
Article
A Comprehensive Study of the Cobalt(II) Chelation Mechanism by an Iminodiacetate-Decorated Disaccharide Ligand
by Cécile Barbot, Laura Gouriou, Mélanie Mignot, Muriel Sebban, Ping Zhang, David Landy, Chang-Chun Ling and Géraldine Gouhier
Molecules 2025, 30(15), 3263; https://doi.org/10.3390/molecules30153263 - 4 Aug 2025
Viewed by 111
Abstract
We report an investigation on the cobalt(II) chelation mechanism by a modified α-maltoside ligand 9 decorated with two iminodiacetate (IDA) residues on C6,C6′ positions. Herein we uncovered the capacity of this biodegradable ligand to chelate cobalt(II), an ionic metal contaminant in the environment [...] Read more.
We report an investigation on the cobalt(II) chelation mechanism by a modified α-maltoside ligand 9 decorated with two iminodiacetate (IDA) residues on C6,C6′ positions. Herein we uncovered the capacity of this biodegradable ligand to chelate cobalt(II), an ionic metal contaminant in the environment that is used, in particular, in lithium-ion batteries. The interactions between cobalt(II) and synthesized ligand 9 were systematically studied using different analytical methods such as 1H and 13C NMR, potentiometry, spectrophotometry, ITC, and ICP-AES. We observed a high affinity for the 1:1 complex, one cobalt(II) associated with two iminodiacetate groups, which is 10-fold higher than the 2:1 complex, where each of the two IDA groups interacts alone with a cobalt(II). Taking into account the log βCoL value obtained (≈12.3) with the stoichiometry 1:1, the strength of this complexation with cobalt(II) can be ranked as follows for the most common ligands: IDA < MIDA < NTA < 9 < EDTA < TTHA < DTPA. We further completed a preliminary remediation test with water contaminated with cobalt(II) and recovered cobalt(II) metal using Chelex® resin, which allowed a recycling of the synthetic ligand for future recovering experiments. The results shed light on the great potential of using this synthetic ligand as an effective and green remediation tool. Full article
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23 pages, 3040 KiB  
Review
All-Solid-State Anode-Free Sodium Batteries: Challenges and Prospects
by Alexander M. Skundin and Tatiana L. Kulova
Batteries 2025, 11(8), 292; https://doi.org/10.3390/batteries11080292 - 2 Aug 2025
Viewed by 326
Abstract
All-solid-state anode-free sodium batteries present a special and especially important kind of energy storage device. Unfortunately, the industrial production of such batteries has been absent up to now, although the prospects of their development seem to be rather optimistic. The present mini review [...] Read more.
All-solid-state anode-free sodium batteries present a special and especially important kind of energy storage device. Unfortunately, the industrial production of such batteries has been absent up to now, although the prospects of their development seem to be rather optimistic. The present mini review considers the fundamental advantages of all-solid-state anode-free sodium batteries as well as challenges in their creation. The advantages of all-solid-state anode-free sodium batteries reveal themselves when comparing them with ordinary sodium-ion batteries, sodium metal batteries, sodium batteries with liquid electrolyte, and their lithium counterparts. Full article
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14 pages, 4979 KiB  
Article
Oxygen Vacancy-Engineered Ni:Co3O4/Attapulgite Photothermal Catalyst from Recycled Spent Lithium-Ion Batteries for Efficient CO2 Reduction
by Jian Shi, Yao Xiao, Menghan Yu and Xiazhang Li
Catalysts 2025, 15(8), 732; https://doi.org/10.3390/catal15080732 - 1 Aug 2025
Viewed by 276
Abstract
Accelerated industrialization and surging energy demands have led to continuously rising atmospheric CO2 concentrations. Developing sustainable methods to reduce atmospheric CO2 levels is crucial for achieving carbon neutrality. Concurrently, the rapid development of new energy vehicles has driven a significant increase [...] Read more.
Accelerated industrialization and surging energy demands have led to continuously rising atmospheric CO2 concentrations. Developing sustainable methods to reduce atmospheric CO2 levels is crucial for achieving carbon neutrality. Concurrently, the rapid development of new energy vehicles has driven a significant increase in demand for lithium-ion batteries (LIBs), which are now approaching an end-of-life peak. Efficient recycling of valuable metals from spent LIBs represents a critical challenge. This study employs conventional hydrometallurgical processing to recover valuable metals from spent LIBs. Subsequently, Ni-doped Co3O4 (Ni:Co3O4) supported on the natural mineral attapulgite (ATP) was synthesized via a sol–gel method. The incorporation of a small amount of Ni into the Co3O4 lattice generates oxygen vacancies, inducing a localized surface plasmon resonance (LSPR) effect, which significantly enhances charge carrier transport and separation efficiency. During the photocatalytic reduction of CO2, the primary product CO generated by the Ni:Co3O4/ATP composite achieved a high production rate of 30.1 μmol·g−1·h−1. Furthermore, the composite maintains robust catalytic activity even after five consecutive reaction cycles. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Air Pollution Control)
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18 pages, 5066 KiB  
Article
Influence of Pulse Duration on Cutting-Edge Quality and Electrochemical Performance of Lithium Metal Anodes
by Lars O. Schmidt, Houssin Wehbe, Sven Hartwig and Maja W. Kandula
Batteries 2025, 11(8), 286; https://doi.org/10.3390/batteries11080286 - 26 Jul 2025
Viewed by 311
Abstract
Lithium metal is a promising anode material for next-generation batteries due to its high specific capacity and low density. However, conventional mechanical processing methods are unsuitable due to lithium’s high reactivity and adhesion. Laser cutting offers a non-contact alternative, but photothermal effects can [...] Read more.
Lithium metal is a promising anode material for next-generation batteries due to its high specific capacity and low density. However, conventional mechanical processing methods are unsuitable due to lithium’s high reactivity and adhesion. Laser cutting offers a non-contact alternative, but photothermal effects can negatively impact the cutting quality and electrochemical performance. This study investigates the influence of pulse duration on the cutting-edge characteristics and electrochemical behavior of laser-cut 20 µm lithium metal on 10 µm copper foils using nanosecond and picosecond laser systems. It was demonstrated that shorter pulse durations significantly reduce the heat-affected zone (HAZ), resulting in improved cutting quality. Electrochemical tests in symmetric Li|Li cells revealed that laser-cut electrodes exhibit enhanced cycling stability compared with mechanically separated anodes, despite the presence of localized dead lithium “reservoirs”. While the overall pulse duration did not show a direct impact on ionic resistance, the characteristics of the cutting edge, particularly the extent of the HAZ, were found to influence the electrochemical performance. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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18 pages, 2688 KiB  
Article
Eco-Friendly Leaching of Spent Lithium-Ion Battery Black Mass Using a Ternary Deep Eutectic Solvent System Based on Choline Chloride, Glycolic Acid, and Ascorbic Acid
by Furkan Nazlı, Işıl Hasdemir, Emircan Uysal, Halide Nur Dursun, Utku Orçun Gezici, Duygu Yesiltepe Özçelik, Fırat Burat and Sebahattin Gürmen
Minerals 2025, 15(8), 782; https://doi.org/10.3390/min15080782 - 25 Jul 2025
Viewed by 416
Abstract
Lithium-ion batteries (LiBs) are utilized in numerous applications due to advancements in technology, and the recovery of end-of-life (EoL) LiBs is imperative for environmental and economic reasons. Pyrometallurgical and hydrometallurgical methods have been used in the recovery of metals such as Li, Co, [...] Read more.
Lithium-ion batteries (LiBs) are utilized in numerous applications due to advancements in technology, and the recovery of end-of-life (EoL) LiBs is imperative for environmental and economic reasons. Pyrometallurgical and hydrometallurgical methods have been used in the recovery of metals such as Li, Co, and Ni in the EoL LiBs. Hydrometallurgical methods, which have been demonstrated to exhibit higher recovery efficiency and reduced energy consumption, have garnered increased attention in recent research. Inorganic acids, including HCl, HNO3, and H2SO4, as well as organic acids such as acetic acid and citric acid, are employed in the hydrometallurgical recovery of these metals. It is imperative to acknowledge the environmental hazards posed by these acids. Consequently, solvometallurgical processes, which involve the use of organic solvents with minimal or no water, are gaining increasing attention as alternative or complementary techniques to conventional hydrometallurgical processes. In the context of solvent systems that have been examined for a range of solvometallurgical methods, deep eutectic solvents (DESs) have garnered particular interest due to their low toxicity, biodegradable nature, tunable properties, and efficient metal recovery potential. In this study, the leaching process of black mass containing graphite, LCO, NMC, and LMO was carried out in a short time using the ternary DES system. The ternary DES system consists of choline chloride (ChCl), glycolic acid (GLY), and ascorbic acid (AA). As a result of the leaching process of cathode powders in the black mass without any pre-enrichment process, Li, Co, Ni, and Mn elements passed into solution with an efficiency of over 95% at 60 °C and within 1 h. Moreover, the kinetics of the leaching process was investigated, and Density Functional Theory (DFT) calculations were used to explain the leaching mechanism. Full article
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18 pages, 4914 KiB  
Article
Preparation and Failure Behavior of Gel Electrolytes for Multilayer Structure Lithium Metal Solid-State Batteries
by Chu Chen, Wendong Qin, Qiankun Hun, Yujiang Wang, Xinghua Liang, Renji Tan, Junming Li and Yifeng Guo
Gels 2025, 11(8), 573; https://doi.org/10.3390/gels11080573 - 23 Jul 2025
Viewed by 284
Abstract
High safety gel polymer electrolyte (GPE) is used in lithium metal solid state batteries, which has the advantages of high energy density, wide temperature range, high safety, and is considered as a subversive new generation battery technology. However, solid-state lithium batteries with multiple [...] Read more.
High safety gel polymer electrolyte (GPE) is used in lithium metal solid state batteries, which has the advantages of high energy density, wide temperature range, high safety, and is considered as a subversive new generation battery technology. However, solid-state lithium batteries with multiple layers and large capacity currently have poor cycle life and a large gap between the actual output cycle capacity retention rate and the theoretical level. In this paper, polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP)/polyacrylonitrile (PAN)—lithium perchlorate (LiClO4)—lithium lanthanum zirconium tantalate (LLZTO) gel polymer electrolytes was prepared by UV curing process using a UV curing machine at a speed of 0.01 m/min for 10 s, with the temperature controlled at 30 °C and wavelength 365 nm. In order to study the performance and failure mechanism of multilayer solid state batteries, single and three layers of solid state batteries with ceramic/polymer composite gel electrolyte were assembled. The results show that the rate and cycle performance of single-layer solid state battery with gel electrolyte are better than those of three-layer solid state battery. As the number of cycles increases, the interface impedance of both single-layer and three-layer electrolyte membrane solid-state batteries shows an increasing trend. Specifically, the three-layer battery impedance increased from 17 Ω to 42 Ω after 100 cycles, while the single-layer battery showed a smaller increase, from 2.2 Ω to 4.8 Ω, indicating better interfacial stability. After 100 cycles, the interface impedance of multi-layer solid-state batteries increases by 9.61 times that of single-layer batteries. After 100 cycles, the corresponding capacity retention rates were 48.9% and 15.6%, respectively. This work provides a new strategy for large capacity solid state batteries with gel electrolyte design. Full article
(This article belongs to the Special Issue Research Progress and Application Prospects of Gel Electrolytes)
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15 pages, 4358 KiB  
Article
Nickel-Rich Cathodes for Solid-State Lithium Batteries: Comparative Study Between PVA and PIB Binders
by José M. Pinheiro, Beatriz Moura Gomes, Manuela C. Baptista and M. Helena Braga
Molecules 2025, 30(14), 2974; https://doi.org/10.3390/molecules30142974 - 15 Jul 2025
Viewed by 403
Abstract
The growing demand for high-energy, safe, and sustainable lithium-ion batteries has increased interest in nickel-rich cathode materials and solid-state electrolytes. This study presents a scalable wet-processing method for fabricating composite cathodes for all-solid-state batteries. The cathodes studied herein are high-nickel LiNi0.90Mn [...] Read more.
The growing demand for high-energy, safe, and sustainable lithium-ion batteries has increased interest in nickel-rich cathode materials and solid-state electrolytes. This study presents a scalable wet-processing method for fabricating composite cathodes for all-solid-state batteries. The cathodes studied herein are high-nickel LiNi0.90Mn0.05Co0.05O2, NMC955, the sulfide-based electrolyte Li6PS5Cl, and alternative binders—polyvinyl alcohol (PVA) and polyisobutylene (PIB)—dispersed in toluene, a non-polar solvent compatible with the electrolyte. After fabrication, the cathodes were characterized using SEM/EDX, sheet resistance, and Hall effect measurements. Electrochemical tests were additionally performed in all-solid-state battery half-cells comprising the synthesized cathodes, lithium metal anodes, and Li6PS5Cl as the separator and electrolyte. The results show that both PIB and PVA formulations yielded conductive cathodes with stable microstructures and uniform particle distribution. Electrochemical characterization exposed that the PVA-based cathode outperformed the PIB-based counterpart, achieving the theoretical capacity of 192 mAh·g−1 even at 1C, whereas the PIB cathode reached a maximum capacity of 145 mAh.g−1 at C/40. Post-mortem analysis confirmed the structural integrity of the cathodes. These findings demonstrate the viability of NMC955 as a high-capacity cathode material compatible with solid-state systems. Full article
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12 pages, 23410 KiB  
Article
Recycling and Separation of Valuable Metals from Spent Cathode Sheets by Single-Step Electrochemical Strategy
by Neng Wei, Yaqun He, Guangwen Zhang, Jiahao Li and Fengbin Zhang
Separations 2025, 12(7), 178; https://doi.org/10.3390/separations12070178 - 5 Jul 2025
Viewed by 284
Abstract
The conventional spent lithium-ion batteries (LIBs) recycling method suffers from complex processes and excessive chemical consumption. Hence, this study proposes an electrochemical strategy for achieving reductant-free leaching of high-valence transition metals and efficient separation of valuable components from spent cathode sheets (CSs). An [...] Read more.
The conventional spent lithium-ion batteries (LIBs) recycling method suffers from complex processes and excessive chemical consumption. Hence, this study proposes an electrochemical strategy for achieving reductant-free leaching of high-valence transition metals and efficient separation of valuable components from spent cathode sheets (CSs). An innovatively designed sandwich-structured electrochemical reactor achieved efficient reductive dissolution of cathode materials (CMs) while maintaining the structural integrity of aluminum (Al) foils in a dilute sulfuric acid system. Optimized current enabled leaching efficiencies exceeding 93% for lithium (Li), cobalt (Co), manganese (Mn), and nickel (Ni), with 88% metallic Al foil recovery via cathodic protection. Multi-scale characterization systematically elucidated metal valence evolution and interfacial reaction mechanisms, validating the technology’s tripartite innovation: simultaneous high metal extraction efficiency, high value-added Al foil recovery, and organic removal through single-step electrochemical treatment. The process synergized the dissolution of CM particles and hydrogen bubble-induced physical liberation to achieve clean separation of polyvinylidene difluoride (PVDF) and carbon black (CB) layers from Al foil substrates. This method eliminates crushing pretreatment, high-temperature reduction, and any other reductant consumption, establishing an environmentally friendly and efficient method of comprehensive recycling of battery materials. Full article
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18 pages, 2187 KiB  
Article
Study of Three-Component Fe2O3/TiO2/rGO Nanocomposite Thin Films Anode for Lithium-Ion Batteries
by Kaspars Kaprans, Gunars Bajars and Gints Kucinskis
Energies 2025, 18(13), 3490; https://doi.org/10.3390/en18133490 - 2 Jul 2025
Viewed by 350
Abstract
In this study, we synthesized anode materials based on iron oxide (Fe2O3), titanium dioxide (TiO2), and reduced graphene oxide (rGO) via the electrophoretic deposition technique. The structural and morphological characteristics of electrodes were examined through various methods [...] Read more.
In this study, we synthesized anode materials based on iron oxide (Fe2O3), titanium dioxide (TiO2), and reduced graphene oxide (rGO) via the electrophoretic deposition technique. The structural and morphological characteristics of electrodes were examined through various methods including SEM, XRD, Raman, and XPS. Among the investigated compositions, the three-component Fe2O3/TiO2/rGO electrode displayed superior electrochemical characteristics in comparison to the binary Fe2O3/rGO and TiO2/rGO electrodes. Specific capacities of 571, 683, and 729 mAh/g were achieved at 0.5 mA for the respective Fe2O3:TiO2 molar ratios of 1:1, 2:1, and 3:1. The 2:1 ratio configuration offered the most promising balance between cycling stability and capacity, highlighting its potential as a high-performance anode in lithium-ion batteries. This work contributes valuable insights into the synergistic behavior of dual-transition metal oxides in composite electrode design using a low-cost and scalable method. Full article
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31 pages, 6211 KiB  
Review
Unlocking the Potential of MBenes in Li/Na-Ion Batteries
by Zixin Li, Yao Hu, Haihui Lan and Huicong Xia
Molecules 2025, 30(13), 2831; https://doi.org/10.3390/molecules30132831 - 1 Jul 2025
Cited by 1 | Viewed by 408
Abstract
MBenes, an emerging family of two-dimensional transition metal boride materials, are gaining prominence in alkali metal-ion battery research owing to their distinctive stratified architecture, enhanced charge transport properties, and exceptional electrochemical durability. This analysis provides a comprehensive examination of morphological characteristics and fabrication [...] Read more.
MBenes, an emerging family of two-dimensional transition metal boride materials, are gaining prominence in alkali metal-ion battery research owing to their distinctive stratified architecture, enhanced charge transport properties, and exceptional electrochemical durability. This analysis provides a comprehensive examination of morphological characteristics and fabrication protocols for MBenes, with particular focus on strategies for optimizing energy storage metrics through controlled adjustment of interlayer distance and tailored surface modifications. The discussion highlights these materials’ unique capability to host substantial alkali metal ions, translating to exceptional longevity during charge–discharge cycling and remarkable high-current performance in both lithium and sodium battery systems. Current obstacles to materials development are critically evaluated, encompassing precision control in nanoscale synthesis, reproducibility in large-scale production, enhancement of thermodynamic stability, and eco-friendly processing requirements. Prospective research pathways are proposed, including sustainable manufacturing innovations, atomic-level structural tailoring through computational modeling, and expansion into hybrid energy storage-conversion platforms. By integrating fundamental material science principles with practical engineering considerations, this work seeks to establish actionable frameworks for advancing MBene-based technologies toward next-generation electrochemical storage solutions with enhanced energy density and operational reliability. Full article
(This article belongs to the Special Issue Carbon-Based Electrochemical Materials for Energy Storage)
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17 pages, 3910 KiB  
Article
Extraction of Valuable Metals from Spent Li-Ion Batteries Combining Reduction Smelting and Chlorination
by Chen Wang, Wei Liu, Congren Yang and Hongbin Ling
Metals 2025, 15(7), 732; https://doi.org/10.3390/met15070732 - 30 Jun 2025
Viewed by 382
Abstract
Pyrometallurgical recycling of lithium-ion batteries presents distinct advantages including streamlined processing, simplified pretreatment requirements, and high throughput capacity. However, its industrial implementation faces challenges associated with high energy demands and lithium loss into slag phases. This investigation develops an integrated reduction smelting–chloridizing volatilization [...] Read more.
Pyrometallurgical recycling of lithium-ion batteries presents distinct advantages including streamlined processing, simplified pretreatment requirements, and high throughput capacity. However, its industrial implementation faces challenges associated with high energy demands and lithium loss into slag phases. This investigation develops an integrated reduction smelting–chloridizing volatilization process for the comprehensive recovery of strategic metals (Li, Mn, Cu, Co, Ni) from spent ternary lithium-ion batteries; calcium chloride was selected as the chlorinating agent for this purpose. Thermodynamic analysis was performed to understand the phase evolution during reduction smelting and to design an appropriate slag composition. Preliminary experiments compared carbon and aluminum powder as reducing agents to identify optimal operational parameters: a smelting temperature of 1450 °C, 2.5 times theoretical CaCl2 dosage, and duration of 120 min. The process achieved effective element partitioning with lithium and manganese volatilizing as chloride species, while transition metals (Cu, Ni, Co) were concentrated into an alloy phase. Process validation in an induction furnace with N2-O2 top blowing demonstrated enhanced recovery efficiency through optimized oxygen supplementation (four times the theoretical oxygen requirement). The recovery rates of Li, Mn, Cu, Co, and Ni reached 94.1%, 93.5%, 97.6%, 94.4%, and 96.4%, respectively. This synergistic approach establishes an energy-efficient pathway for simultaneous multi-metal recovery, demonstrating industrial viability for large-scale lithium-ion battery recycling through minimized processing steps and maximized resource utilization. Full article
(This article belongs to the Special Issue Green Technologies in Metal Recovery)
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18 pages, 1972 KiB  
Article
Lithium Growth on Alloying Substrates and Effect on Volumetric Expansion
by Laura C. Merrill, Robert L. Craig, Damion P. Cummings and Julia I. Deitz
Batteries 2025, 11(7), 249; https://doi.org/10.3390/batteries11070249 - 29 Jun 2025
Viewed by 350
Abstract
The widespread implementation of next-generation Li metal anodes is limited, in part, due to the formation of dendritic and/or mossy electrodeposits during cycling. These morphologies can lead to battery failure due to the formation of short circuits and significant volumetric expansion at the [...] Read more.
The widespread implementation of next-generation Li metal anodes is limited, in part, due to the formation of dendritic and/or mossy electrodeposits during cycling. These morphologies can lead to battery failure due to the formation of short circuits and significant volumetric expansion at the anode. One strategy to control the electrodeposition of Li metal is to use lithiophilic materials at the anode. Here, we evaluate the impact of Ag and Au on the early stages of Li metal electrodeposition and cycling. The alloying substrates decrease the voltage for Li reduction and improve Li wetting/adhesion. We probe volumetric expansion directly through dilatometry measurements and find that the degree of volumetric expansion is less when lithium is cycled on an alloying substrate compared to a non-alloying substrate (Cu). Dilatometry experiments reveal that Au has the least amount of volumetric expansion and coin cell cycling experiments indicate that Ag yields more stable cycling compared to Au or Cu. The evaluation of in situ cross-sectional images of cycled coin cells shows that Ag has the lowest volumetric expansion in a coin cell format. Full article
(This article belongs to the Special Issue Batteries: 10th Anniversary)
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14 pages, 2161 KiB  
Article
Observation of Electroplating in a Lithium-Metal Battery Model Using Magnetic Resonance Microscopy
by Rok Peklar, Urša Mikac and Igor Serša
Molecules 2025, 30(13), 2733; https://doi.org/10.3390/molecules30132733 - 25 Jun 2025
Viewed by 381
Abstract
Accurate imaging methods are important for understanding electrodeposition phenomena in metal batteries. Among the suitable imaging methods for this task is magnetic resonance imaging (MRI), which is a very powerful radiological diagnostic method. In this study, MR microscopy was used to image electroplating [...] Read more.
Accurate imaging methods are important for understanding electrodeposition phenomena in metal batteries. Among the suitable imaging methods for this task is magnetic resonance imaging (MRI), which is a very powerful radiological diagnostic method. In this study, MR microscopy was used to image electroplating in a lithium symmetric cell, which was used as a model for a lithium-metal battery. Lithium electrodeposition in this cell was studied by sequential 3D 1H MRI of 1 M LiPF6 in EC/DMC electrolyte under different charging conditions, which resulted in different dynamics of the amount of electroplated lithium and its structure. The acquired images depicted the electrolyte distribution, so that the images of deposited lithium that did not give a detectable signal corresponded to the negatives of these images. With this indirect MRI, phenomena such as the transition from a mossy to a dendritic structure at Sand’s time, the growth of whiskers, the growth of dendrites with arborescent structure, the formation of dead lithium, and the formation of gas due to electrolyte decomposition were observed. In addition, the effect of charge and discharge cycles on electrodeposition was also studied. It was found that it is difficult to correctly predict the occurrence of these phenomena based on charging conditions alone, as seemingly identical conditions resulted in different results. Full article
(This article belongs to the Special Issue Advanced Magnetic Resonance Methods in Materials Chemistry Analysis)
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15 pages, 1787 KiB  
Article
Probing Solid-State Interface Kinetics via Alternating Current Electrophoretic Deposition: LiFePO4 Li-Metal Batteries
by Su Jeong Lee and Byoungnam Park
Appl. Sci. 2025, 15(13), 7120; https://doi.org/10.3390/app15137120 - 24 Jun 2025
Viewed by 337
Abstract
This work presents a comprehensive investigation into the interfacial charge storage mechanisms and lithium-ion transport behavior of Li-metal all-solid-state batteries (ASSBs) employing LiFePO4 (LFP) cathodes fabricated via alternating current electrophoretic deposition (AC-EPD) and Li1.3Al0.3Ti1.7(PO4) [...] Read more.
This work presents a comprehensive investigation into the interfacial charge storage mechanisms and lithium-ion transport behavior of Li-metal all-solid-state batteries (ASSBs) employing LiFePO4 (LFP) cathodes fabricated via alternating current electrophoretic deposition (AC-EPD) and Li1.3Al0.3Ti1.7(PO4)3 (LATP) as the solid-state electrolyte. We demonstrate that optimal sintering improves the LATP–LFP interfacial contact, leading to higher lithium diffusivity (~10−9 cm2∙s−1) and diffusion-controlled kinetics (b ≈ 0.5), which directly translate to better rate capability. Structural and electrochemical analyses—including X-ray diffraction, scanning electron microscopy, cyclic voltammetry, and rate capability tests—demonstrate that the cell with LATP sintered at 900 °C delivers the highest Li-ion diffusivity (~10−9 cm2∙s−1), near-ideal diffusion-controlled behavior (b-values ~0.5), and superior rate capability. In contrast, excessive sintering at 1000 °C led to reduced diffusivity (~10−10 cm2∙s−1). The liquid electrolyte system showed higher b-values (~0.58), indicating the inclusion of surface capacitive behavior. The correlation between b-values, diffusivity, and morphology underscores the critical role of interface engineering and electrolyte processing in determining the performance of solid-state batteries. This study establishes AC-EPD as a viable and scalable method for fabricating additive-free LFP cathodes and offers new insights into the structure–property relationships governing the interfacial transport in ASSBs. Full article
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