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46 pages, 1449 KB  
Review
MXenes in Solid-State Batteries: Multifunctional Roles from Electrodes to Electrolytes and Interfacial Engineering
by Francisco Márquez
Batteries 2025, 11(10), 364; https://doi.org/10.3390/batteries11100364 - 2 Oct 2025
Abstract
MXenes, a rapidly emerging family of two-dimensional transition metal carbides and nitrides, have attracted considerable attention in recent years for their potential in next-generation energy storage technologies. In solid-state batteries (SSBs), they combine metallic-level conductivity (>103 S cm−1), adjustable surface [...] Read more.
MXenes, a rapidly emerging family of two-dimensional transition metal carbides and nitrides, have attracted considerable attention in recent years for their potential in next-generation energy storage technologies. In solid-state batteries (SSBs), they combine metallic-level conductivity (>103 S cm−1), adjustable surface terminations, and mechanical resilience, which makes them suitable for diverse functions within the cell architecture. Current studies have shown that MXene-based anodes can deliver reversible lithium storage with Coulombic efficiencies approaching ~98% over 500 cycles, while their use as conductive additives in cathodes significantly improves electron transport and rate capability. As interfacial layers or structural scaffolds, MXenes effectively buffer volume fluctuations and suppress lithium dendrite growth, contributing to extended cycle life. In solid polymer and composite electrolytes, MXene fillers have been reported to increase Li+ conductivity to the 10−3–10−2 S cm−1 range and enhance Li+ transference numbers (up to ~0.76), thereby improving both ionic transport and mechanical stability. Beyond established Ti-based systems, double transition metal MXenes (e.g., Mo2TiC2, Mo2Ti2C3) and hybrid heterostructures offer expanded opportunities for tailoring interfacial chemistry and optimizing energy density. Despite these advances, large-scale deployment remains constrained by high synthesis costs (often exceeding USD 200–400 kg−1 for Ti3C2Tx at lab scale), restacking effects, and stability concerns, highlighting the need for greener etching processes, robust quality control, and integration with existing gigafactory production lines. Addressing these challenges will be crucial for enabling MXene-based SSBs to transition from laboratory prototypes to commercially viable, safe, and high-performance energy storage systems. Beyond summarizing performance, this review elucidates the mechanistic roles of MXenes in SSBs—linking lithiophilicity, field homogenization, and interphase formation to dendrite suppression at Li|SSE interfaces, and termination-assisted salt dissociation, segmental-motion facilitation, and MWS polarization to enhanced electrolyte conductivity—thereby providing a clear design rationale for practical implementation. Full article
(This article belongs to the Collection Feature Papers in Batteries)
18 pages, 1972 KB  
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 572
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 KB  
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 588
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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29 pages, 4963 KB  
Review
Protective Layer and Current Collector Design for Interface Stabilization in Lithium-Metal Batteries
by Dayoung Kim, Cheolhwan Song and Oh B. Chae
Batteries 2025, 11(6), 220; https://doi.org/10.3390/batteries11060220 - 5 Jun 2025
Viewed by 2078
Abstract
Recent advancements in lithium-metal-based battery technology have garnered significant attention, driven by the increasing demand for high-energy storage devices such as electric vehicles (EVs). Lithium (Li) metal has long been considered an ideal negative electrode due to its high theoretical specific capacity (3860 [...] Read more.
Recent advancements in lithium-metal-based battery technology have garnered significant attention, driven by the increasing demand for high-energy storage devices such as electric vehicles (EVs). Lithium (Li) metal has long been considered an ideal negative electrode due to its high theoretical specific capacity (3860 mAh g−1) and low redox potential. However, the commercialization of Li-metal batteries (LMBs) faces significant challenges, primarily related to the safety and cyclability of the negative electrodes. The formation of lithium dendrites and uneven solid electrolyte interphases, along with volumetric expansion during cycling, severely hinder the commercial viability of LMBs. Among the various strategies developed to overcome these challenges, the introduction of artificial protective layers and the structural engineering of current collectors have emerged as highly promising approaches. These techniques are critical for regulating Li deposition behavior, mitigating dendrite growth, and enhancing interfacial and mechanical stability. This review summarizes the current state of Li-negative electrodes and introduces methods of enhancing their performance using a protective layer and current collector design. Full article
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65 pages, 11913 KB  
Review
MXenes and MXene-Based Composites: Preparation, Characteristics, Theoretical Investigations, and Application in Developing Sulfur Cathodes, Lithium Anodes, and Functional Separators for Lithium–Sulfur Batteries
by Narasimharao Kitchamsetti, Hyuksu Han and Sungwook Mhin
Batteries 2025, 11(6), 206; https://doi.org/10.3390/batteries11060206 - 23 May 2025
Viewed by 1923
Abstract
Lithium–sulfur batteries (LSBs) are favorable candidates for advanced energy storage, boasting a remarkable theoretical energy density of 2600 Wh kg−1. Moreover, several challenges hinder their practical implementation, including sulfur’s intrinsic electrical insulation, the shuttle effect of lithium polysulfides (LiPSs), sluggish redox [...] Read more.
Lithium–sulfur batteries (LSBs) are favorable candidates for advanced energy storage, boasting a remarkable theoretical energy density of 2600 Wh kg−1. Moreover, several challenges hinder their practical implementation, including sulfur’s intrinsic electrical insulation, the shuttle effect of lithium polysulfides (LiPSs), sluggish redox kinetics of Li2S2/Li2S, and the uncontrolled growth of Li dendrites. These issues pose significant obstacles to the commercialization of LSBs. A viable strategy to address these challenges involves using MXene materials, 2D transition metal carbides, and nitrides (TMCs/TMNs) as hosts, functional separators, or interlayers. MXenes offer exceptional electronic conductivity, adjustable structural properties, and abundant polar functional groups, enabling strong interactions with both S cathodes and Li anodes. Despite their advantages, current MXene synthesis methods predominantly rely on acid etching, which is associated with environmental concerns, low production efficiency, and limited structural versatility, restricting their potential in LSBs. This review provides a comprehensive overview of traditional and environmentally sustainable MXene synthesis techniques, emphasizing their applications in developing S cathodes, Li anodes, and functional separators for LSBs. Additionally, it discusses the challenges and outlines future directions for advancing MXene-based solutions in LSBs technology. Full article
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13 pages, 3626 KB  
Article
Lithiophilic Modification of Self-Supporting Carbon-Based Hosts and Lithium Metal Plating/Stripping Behaviors
by Zipeng Jiang, Shoudong Xie, Guijun Yang, Huiyuan Chen, Jiahang Lv, Ang Li, Chengwei Fan and Huaihe Song
Nanomaterials 2025, 15(10), 746; https://doi.org/10.3390/nano15100746 - 15 May 2025
Viewed by 526
Abstract
Metallic lithium anodes possess the lowest redox potential (−3.04 V vs. SHE) and an ultra-high theoretical capacity (3860 mAh g−1, 2061 mAh cm−3). However, during electrochemical cycling, lithium metal tends to plate unevenly, leading to the formation of lithium [...] Read more.
Metallic lithium anodes possess the lowest redox potential (−3.04 V vs. SHE) and an ultra-high theoretical capacity (3860 mAh g−1, 2061 mAh cm−3). However, during electrochemical cycling, lithium metal tends to plate unevenly, leading to the formation of lithium dendrites. Moreover, severe electrochemical corrosion occurs at the interface between metallic lithium and traditional copper foil current collectors. To address these issues, we selected corrosion-resistant carbon paper as a lithium metal host and modified a uniform distribution of silver nanoparticles and a F-doped amorphous carbon structure as a highly lithiophilic F-CP@Ag host to enhance lithium-ion transport kinetics and achieve improved affinity with lithium metal. The silver nanoparticles reduced the lithium nucleation energy barrier, while F doping resulted in a LiF-rich solid electrolyte interphase that better accommodated volume changes in lithium metal. These two strategies worked together to ensure uniform and stable lithium metal plating/stripping on the F-CP@Ag host. Consequently, under the conditions of 1 mA cm−2 and 1 mAh cm−2, the symmetric cell exhibited stable cycling with a polarization voltage of 8 mV for up to 1400 h. This work highlights the corrosion problem of lithium metal on traditional copper foil current collectors and provides guidance for the long-term cycling stability of lithium metal anodes. Full article
(This article belongs to the Section Energy and Catalysis)
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15 pages, 5965 KB  
Article
Gel Polymer Electrolytes with High Thermal Stability for Safe Lithium Metal Batteries
by Xianhui Chen, Xue Wang, Xing Li and Xing Xin
Colloids Interfaces 2025, 9(3), 30; https://doi.org/10.3390/colloids9030030 - 14 May 2025
Viewed by 1477
Abstract
The poor thermal stability of polypropylene (PP) separators poses risks of electrolyte leakage and battery short-circuiting, limiting their application in lithium metal batteries (LMBs). To address these challenges, a gel polymer membrane was designed using polymer blending technology. This membrane effectively retains the [...] Read more.
The poor thermal stability of polypropylene (PP) separators poses risks of electrolyte leakage and battery short-circuiting, limiting their application in lithium metal batteries (LMBs). To address these challenges, a gel polymer membrane was designed using polymer blending technology. This membrane effectively retains the electrolyte, provides a stable environment, enhances thermal stability, and significantly decreases the risk of battery explosions and side reactions between the lithium metal and the electrolyte. Compared to commercial PP separators, the developed blend-type gel polymer electrolyte (b-GPE) demonstrates a superior performance, including structural stability at temperatures up to 150 °C and a high lithium-ion transference number (tLi+) of 0.513. Furthermore, a cell with a LiCoO2 cathode operated at a 1 C rate retains 97.4% of its capacity after 300 cycles. After exposure to 120 °C, the b-GPE-120 demonstrates that its performance is comparable to that of the b-GPE, such as a tLi+ of 0.506, a high electrolyte absorption rate, and a wide electrochemical window of 5.2 V. Full article
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8 pages, 2287 KB  
Communication
Lithiophilic Interlayer with Electrolyte-Reservoir and Dendrite-Buffer for High-Performance Lithium Metal Batteries
by Huasen Shen, Guoning Wu, Tingting Ma, Mengjun Li, Yunan Tian, Si Chen, Shaojun Cai and Zhaohuai Li
Nanomaterials 2025, 15(10), 710; https://doi.org/10.3390/nano15100710 - 9 May 2025
Viewed by 682
Abstract
Uneven local electric fields and limited nucleation sites at the reaction interface can lead to the formation of hazardous lithium (Li) dendrites, posing a significant safety risk and impeding the practical utilization of Li metal anodes (LMAs). Here, we present a method utilizing [...] Read more.
Uneven local electric fields and limited nucleation sites at the reaction interface can lead to the formation of hazardous lithium (Li) dendrites, posing a significant safety risk and impeding the practical utilization of Li metal anodes (LMAs). Here, we present a method utilizing atomic layer deposition (ALD) to create lithiophilic titanium nitride (TiN) sites on carbon nanotubes (CNTs) surfaces, integrated with nanocellulose to form a lithiophilic interlayer (NFCP@TN). This interlayer, which is highly flexible and electrolyte-wettable, functions as a current collector and host material for LMAs. The uniform deposition of Li is facilitated by the synergistic interplay of the lithiophilic active sites TiN, the conductive CNT network, and excellent electrolyte wettability of nanocellulose. As a result, Li preferentially adsorbs on TiN sheaths with lower diffusion barriers, leading to controlled nucleation sites and dendrite-free Li deposition. Furthermore, the well-designed NFCP@TN interlayer exhibits exceptional electrochemical performance and significantly extended cycle life when paired LMA with high areal capacity NCM811 (5.0 mAh cm−2) electrodes. Full article
(This article belongs to the Special Issue Design of Nanomaterials for Electrochemical Devices)
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34 pages, 8692 KB  
Review
Recent Advances in Polyphenylene Sulfide-Based Separators for Lithium-Ion Batteries
by Lianlu Wan, Haitao Zhou, Haiyun Zhou, Jie Gu, Chen Wang, Quan Liao, Hongquan Gao, Jianchun Wu and Xiangdong Huo
Polymers 2025, 17(9), 1237; https://doi.org/10.3390/polym17091237 - 30 Apr 2025
Viewed by 1389
Abstract
Polyphenylene sulfide (PPS)-based separators have garnered significant attention as high-performance components for next-generation lithium-ion batteries (LIBs), driven by their exceptional thermal stability (>260 °C), chemical inertness, and mechanical durability. This review comprehensively examines advances in PPS separator design, focusing on two structurally distinct [...] Read more.
Polyphenylene sulfide (PPS)-based separators have garnered significant attention as high-performance components for next-generation lithium-ion batteries (LIBs), driven by their exceptional thermal stability (>260 °C), chemical inertness, and mechanical durability. This review comprehensively examines advances in PPS separator design, focusing on two structurally distinct categories: porous separators engineered via wet-chemical methods (e.g., melt-blown spinning, electrospinning, thermally induced phase separation) and nonporous solid-state separators fabricated through solvent-free dry-film processes. Porous variants, typified by submicron pore architectures (<1 μm), enable electrolyte-mediated ion transport with ionic conductivities up to >1 mS·cm−1 at >55% porosity, while their nonporous counterparts leverage crystalline sulfur-atom alignment and trace electrolyte infiltration to establish solid–liquid biphasic conduction pathways, achieving ion transference numbers >0.8 and homogenized lithium flux. Dry-processed solid-state PPS separators demonstrate unparalleled thermal dimensional stability (<2% shrinkage at 280 °C) and mitigate dendrite propagation through uniform electric field distribution, as evidenced by COMSOL simulations showing stable Li deposition under Cu particle contamination. Despite these advancements, challenges persist in reconciling thickness constraints (<25 μm) with mechanical robustness, scaling solvent-free manufacturing, and reducing costs. Innovations in ultra-thin formats (<20 μm) with self-healing polymer networks, coupled with compatibility extensions to sodium/zinc-ion systems, are identified as critical pathways for advancing PPS separators. By addressing these challenges, PPS-based architectures hold transformative potential for enabling high-energy-density (>500 Wh·kg−1), intrinsically safe energy storage systems, particularly in applications demanding extreme operational reliability such as electric vehicles and grid-scale storage. Full article
(This article belongs to the Section Polymer Applications)
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21 pages, 4601 KB  
Article
Artificial Interfacial Layers with Zwitterionic Ion Structure Improves Lithium Symmetric Battery Life and Inhibits Dendrite Growth
by Haihua Wang, Wei Yuan, Chaoxian Chen, Rui Cao, Huizhu Niu, Ling Song, Jie Wang and Xinyu Shang
Symmetry 2025, 17(5), 652; https://doi.org/10.3390/sym17050652 - 25 Apr 2025
Viewed by 931
Abstract
Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose [...] Read more.
Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose significant challenges to the widespread commercialization of Li metal anodes. We introduce the creation of a hydrogen bond network solid electrolyte interphase (SEI) film that integrates zwitterionic groups, designed to facilitate the stability and longevity of lithium metal batteries (LMBs). Here, we design a PVA/P(SBMA-MBA) hydrogen bond network film (PSM) as an artificial SEI, integrating zwitterions and polyvinyl alcohol (PVA) to synergistically regulate Li⁺ flux. The distinctive zwitterionic effect in the network amplifies the SEI film’s ionic conductivity to 1.14 × 10−4 S cm−1 and attains an impressive Li+ ion transfer number of 0.84. In situ Raman spectroscopy reveals dynamic hydrogen bond reconfiguration under strain, endowing the SEI with self-adaptive mechanical robustness. These properties facilitate a homogeneous Li flux and exceptionally suppress dendritic growth. The advanced Li metal anode may endure over 1200 h at 1 mA cm−2 current density and 1 mAh cm−2 area capacity in a Li|Li symmetric battery. And in full cells paired with LiFePO4 cathodes, 93.8% capacity retention is reached after 300 cycles at 1C. Consequently, this work provides a universal strategy for designing dynamic interphases through molecular dipole engineering, paving the way for safe and durable lithium metal batteries. Full article
(This article belongs to the Section Engineering and Materials)
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14 pages, 11366 KB  
Article
A Lithiophilic Artificial Li3P Interphase with High Li-Ion Conductivity via Solid-State Friction for Lithium Metal Anodes
by Haoling Liu, Wen Pan, Bo Xiao, Yunke Jin, Kun Li, An Wang, Huimiao Li, Zhibin Wu, Yuejiao Chen, Shaozhen Huang, Lin Mei and Libao Chen
Materials 2025, 18(9), 1930; https://doi.org/10.3390/ma18091930 - 24 Apr 2025
Viewed by 695
Abstract
Interfacial modification strategies for lithium metal anodes have emerged as a promising method to improve cycling stability, suppress lithium dendrite growth, and increase Coulombic efficiency. However, the reported chemical synthesis methods lead to side reactions and side products, which hinder their electrochemical performance. [...] Read more.
Interfacial modification strategies for lithium metal anodes have emerged as a promising method to improve cycling stability, suppress lithium dendrite growth, and increase Coulombic efficiency. However, the reported chemical synthesis methods lead to side reactions and side products, which hinder their electrochemical performance. In this study, we propose a novel and facile red phosphorus-assisted solid-state friction method to in situ fabricate a uniform Li3P interphase directly on the surface of lithium metal. Interestingly, the as-formed artificial Li3P interphase with high ionic conductivity and lithium affinity features significantly enhanced interfacial stability and electrochemical kinetics. The symmetric cells based on Li@P with the Li3P interphase achieved a prolonged lifespan, over 1000 h, at 1 mA/cm2 with low polarization. When paired with a high-loading LiFePO4 cathode (10.5 mg/cm2), the Li@P||LiFePO4 full cell retained 88.9% of its capacity after stable cycling for 550 cycles at 2 C and further demonstrated the excellent performance and stability of the Li@P‖LiCoO2 full pouch cell. This study provides an efficient and scalable strategy for stabilizing lithium metal anodes, expanding new ideas for the development of next-generation high-energy-density batteries. Full article
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22 pages, 2941 KB  
Article
Looking Beyond Lithium for Breakthroughs in Magnesium-Ion Batteries as Sustainable Solutions
by Idowu O. Malachi, Adebukola O. Olawumi, Samuel O. Afolabi and B. I. Oladapo
Sustainability 2025, 17(9), 3782; https://doi.org/10.3390/su17093782 - 22 Apr 2025
Cited by 4 | Viewed by 2029
Abstract
The increasing demand for sustainable and cost-effective battery technologies in electric vehicles (EVs) has driven research into alternatives to lithium-ion (Li-ion) batteries. This study investigates magnesium-ion (Mg-ion) batteries as a potential solution, focusing on their energy density, cycle stability, safety, and scalability. The [...] Read more.
The increasing demand for sustainable and cost-effective battery technologies in electric vehicles (EVs) has driven research into alternatives to lithium-ion (Li-ion) batteries. This study investigates magnesium-ion (Mg-ion) batteries as a potential solution, focusing on their energy density, cycle stability, safety, and scalability. The research employs a comprehensive methodology, combining electrochemical testing and simulation models, to analyse magnesium-based anodes, sulphur-based cathodes, and advanced electrolytes such as HMDS2Mg. Key findings reveal that Mg-ion batteries achieve a practical energy density of 500–1000 mAh/g, comparable to high-performance Li-ion systems. With sulphur–graphene cathodes, Mg-ion batteries demonstrated 92% capacity retention after 500 cycles, a 10% improvement over standard configurations. Ionic conductivity reached 1.2 × 10−2 S/cm using HMDS2Mg electrolytes, significantly reducing passivation layer growth to 5 nm after 100 cycles, outperforming Grignard-based systems by 30%. However, the research identified a 15% reduction in charge–discharge efficiency compared to Li-ion batteries due to slower ion diffusion kinetics. This study highlights the safety advantage of magnesium-ion batteries, which eliminate dendrite formation and reduce thermal runaway risks by 40%. These findings position Mg-ion batteries as a promising, sustainable alternative for EVs, emphasising the need for further optimisation in scalability and efficiency. Full article
(This article belongs to the Special Issue Renewable Energy Conversion and Sustainable Power Systems Engineering)
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14 pages, 17658 KB  
Article
MOF-Derived Hollow Dodecahedral Carbon Structures with Abundant N Sites and Co Nanoparticle-Modified Cu Foil for Dendrite-Free Lithium Metal Battery
by Fei Wang, Huijie Wei, Xinyuan Ren, Junle Zhang, Aiyun Jiang, Yong Liu and Fengzhang Ren
Coatings 2025, 15(4), 490; https://doi.org/10.3390/coatings15040490 - 20 Apr 2025
Viewed by 640
Abstract
In this work, hollow dodecahedral carbon structures with abundant N-doping sites and metal nanoparticles (NC-Co-CNTs) based on MOF-derivative materials were designed and prepared as host materials for lithium metal to ensure uniform lithium deposition on a Cu current collector. NC-Co-CNTs have good electrical [...] Read more.
In this work, hollow dodecahedral carbon structures with abundant N-doping sites and metal nanoparticles (NC-Co-CNTs) based on MOF-derivative materials were designed and prepared as host materials for lithium metal to ensure uniform lithium deposition on a Cu current collector. NC-Co-CNTs have good electrical conductivity, which ensures fast electron transport and Li+ transfer. The carbon nanotubes catalytically derived by Co can promote the uniform distribution of Li+ along the hollow dodecahedral carbon surface and deposition inside the cavity, and the larger electronegativity of N-doped sites and lithophilic sites such as Co nanoparticles can effectively adsorb lithium, inducing the Li+ to be deposited in the form of spherical lithium in a dendrite-free state, inhibiting the growth of dendritic lithium and improving the electrochemical performance of the lithium metal battery. Based on the above advantages, the electrodes of NC-Co-CNT-based symmetric cells present superior cycling performance for more than 1100 h with low overpotential at 1 mAh cm−2/1 mAh·cm−2. Even cycling at high current density of 5 mA cm−2 and high deposition parameters of 5 mAh cm−2, it still cycles for up to 800 h at a relatively low overpotential. Full article
(This article belongs to the Special Issue Multilayer Coatings for Nanomaterials: From Synthesis to Applications)
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21 pages, 18354 KB  
Article
On the Morphological Evolution with Cycling of a Ball-Milled Si Slag-Based Electrode for Li-Ion Batteries
by Alexandre Heitz, Victor Vanpeene, Samuel Quéméré, Natalie Herkendaal, Thierry Douillard, Isaac Martens, Marta Mirolo and Lionel Roué
Batteries 2025, 11(4), 151; https://doi.org/10.3390/batteries11040151 - 11 Apr 2025
Viewed by 876
Abstract
A Si/SiC/SiO2 (53/44/3 wt.%) composite is evaluated as an anode material for Li-ion batteries. This material, a result of the high-energy ball-milling of a by-product of the carbothermal reduction of silica (Si slag), is predominantly made up of micrometric particles of amorphous [...] Read more.
A Si/SiC/SiO2 (53/44/3 wt.%) composite is evaluated as an anode material for Li-ion batteries. This material, a result of the high-energy ball-milling of a by-product of the carbothermal reduction of silica (Si slag), is predominantly made up of micrometric particles of amorphous or short-range order Si in which submicrometric SiC inclusions are dispersed. Its capacity is 860 mAh g−1 (1.7 mAh cm−2) after 200 cycles in half-cell configuration and 1.6 mAh cm−2 after 70 cycles in full-cell. The SiC component is not electroactive for lithiation but plays a key role in the electrode stability by preventing the formation of the c-Li15Si4 phase, known to accelerate electrode degradation. It is shown that capacity decay with cycling mainly originates from solid electrolyte interphase (SEI) growth rather than particle disconnections. Complementary wide angle X-ray scattering (WAXS) analyses confirm the SEI grows alongside cycling and allows for the highlighting of its major components, namely, Li2CO3 and LiF. The morphological evolution of the electrode upon cycling is studied by electrochemical dilatometry, operando optical microscopy, and focused ion beam (FIB) and broad ion beam (BIB) scanning electron microscopy (SEM). No particle cracking is observed. However, reconstructed 3D imaging of the electrodes before and after 10 and 200 cycles clearly shows that the particles progressively evolve a dendritic structure. The SEI grows on and within the particles and induces a significant decrease in the electrode’s porosity and an increase in its thickness. Full article
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41 pages, 9104 KB  
Review
Progress in Modeling and Applications of Solid Electrolyte Interphase Layers for Lithium Metal Anodes
by Zhicong Wei, Weitao Zheng, Yijuan Li and Shaoming Huang
Nanomaterials 2025, 15(7), 554; https://doi.org/10.3390/nano15070554 - 5 Apr 2025
Viewed by 1806
Abstract
The increasing demand for high-specific-energy lithium batteries has stimulated extensive research on the lithium metal anode owing to its high specific capacity and low electrode potential. However, the lithium metal will irreversibly react with the electrolyte during the first cycling process, forming an [...] Read more.
The increasing demand for high-specific-energy lithium batteries has stimulated extensive research on the lithium metal anode owing to its high specific capacity and low electrode potential. However, the lithium metal will irreversibly react with the electrolyte during the first cycling process, forming an uneven and unstable solid electrolyte interphase (SEI) layer, which results in the non-uniform deposition of Li ions and thus the formation of lithium dendrites. This could cause a battery short circuit, resulting in safety hazards such as thermal runaway. In addition, the continuous rupture and repair of the SEIs during the repeated charge/discharge processes will constantly consume the active lithium, which leads to a significant decrease in battery capacity. An effective strategy to address these challenges is to design and construct ideal artificial SEIs on the surface of the lithium metal anode. This review analyzes and summarizes the mathematical modeling of SEI, the functional characteristics of SEIs with different components, and finally discusses the challenges faced by artificial SEIs in practical applications of lithium metal batteries and future development directions. Full article
(This article belongs to the Special Issue 2D Materials for Energy Conversion and Storage)
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