Search Results (190)

Solid-state lithium batteries (SSLBs) have emerged as a promising alternative to conventional lithium-ion systems due to their superior safety profile, higher energy density, and potential compatibility with lithium metal anodes. However, a major challenge hindering their widespread deployment is the formation and growth of lithium dendrites, which compromise both performance and safety. This review provides a comprehensive and structured overview of recent advances in dendrite suppression strategies, with special emphasis on the role played by the nature of the solid electrolyte. In particular, we examine suppression mechanisms and material innovations within the three main classes of solid electrolytes: sulfide-based, oxide-based, and polymer-based systems. Each electrolyte class presents distinct advantages and challenges in relation to dendrite behavior. Sulfide electrolytes, known for their high ionic conductivity and good interfacial wettability, suffer from poor mechanical strength and chemical instability. Oxide electrolytes exhibit excellent electrochemical stability and mechanical rigidity but often face high interfacial resistance. Polymer electrolytes, while mechanically flexible and easy to process, generally have lower ionic conductivity and limited thermal stability. This review discusses how these intrinsic properties influence dendrite nucleation and propagation, including the role of interfacial stress, grain boundaries, void formation, and electrochemical heterogeneity. To mitigate dendrite formation, we explore a variety of strategies including interfacial engineering (e.g., the use of artificial interlayers, surface coatings, and chemical additives), mechanical reinforcement (e.g., incorporation of nanostructured or gradient architectures, pressure modulation, and self-healing materials), and modifications of the solid electrolyte and electrode structure. Additionally, we highlight the critical role of advanced characterization techniques—such as in situ electron microscopy, synchrotron-based X-ray diffraction, vibrational spectroscopy, and nuclear magnetic resonance (NMR)—for elucidating dendrite formation mechanisms and evaluating the effectiveness of suppression strategies in real time. By integrating recent experimental and theoretical insights across multiple disciplines, this review identifies key limitations in current approaches and outlines emerging research directions. These include the design of multifunctional interphases, hybrid electrolytes, and real-time diagnostic tools aimed at enabling the development of reliable, scalable, and dendrite-free SSLBs suitable for practical applications in next-generation energy storage. Full article

Over the past few decades, lithium-ion batteries (LIBs) have gained significant attention due to their inherent potential for environmental sustainability and unparalleled energy storage efficiency. Meanwhile, polymer electrolytes have gained popularity in several fields due to their ability to adapt to various battery geometries, enhanced safety features, greater thermal stability, and effectiveness in reducing dendrite growth on the anode. However, their relatively low ionic conductivity compared to liquid electrolytes has limited their application in high-performance devices. This limitation has led to recent studies revolving around the development of poly(ionic liquids) (PILs), particularly imidazolium-mediated polymer backbones as novel electrolyte materials, which can increase the conductivity with fine-tuning structural benefits, while maintaining the advantages of both solid and gel electrolytes. In this study, a curated dataset of 120 data points representing eight different polymers was used to predict ionic conductivity in imidazolium-based PILs as well as the emerging ionene substructures. For this purpose, four ML models: CatBoost, Random Forest, XGBoost, and LightGBM were employed by incorporating chemical structure and temperature as the models’ inputs. The best-performing model was further employed to estimate the conductivity of novel ionenes, offering insights into the potential of advanced polymer architectures for next-generation LIB electrolytes. This approach provides a cost-effective and intelligent pathway to accelerate the design of high-performance electrolyte materials. Full article

The development of high-performance solid electrolytes is critical to advancing solid-state lithium-ion batteries (SSBs), with lithium lanthanum zirconium oxide (LLZO) emerging as a leading candidate due to its chemical stability and wide electrochemical window. In this study, we systematically investigated the effects of cation dopants, including aluminum (Al³⁺), tantalum (Ta⁵⁺), gallium (Ga³⁺), and rubidium (Rb⁺), on the structural, electronic, and ionic transport properties of LLZO using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. It appeared that, among all simulated results, Al-LLZO exhibits the highest ionic conductivity of 1.439 × 10⁻² S/cm with reduced activation energy of 0.138 eV, driven by enhanced lithium vacancy concentrations and preserved cubic-phase stability. Ta-LLZO follows, with a conductivity of 7.12 × 10⁻³ S/cm, while Ga-LLZO and Rb-LLZO provide moderate conductivity of 3.73 × 10⁻³ S/cm and 3.32 × 10⁻³ S/cm, respectively. Charge density analysis reveals that Al and Ta dopants facilitate smoother lithium-ion migration by minimizing electrostatic barriers. Furthermore, Al-LLZO demonstrates low electronic conductivity (1.72 × 10⁻⁸ S/cm) and favorable binding energy, mitigating dendrite formation risks. Comparative evaluations of radial distribution functions (RDFs) and XRD patterns confirm the structural integrity of doped systems. Overall, Al emerges as the most effective and economically viable dopant, optimizing LLZO for scalable, durable, and high-conductivity solid-state batteries. Full article

Lithium lanthanum titanate (LLTO) is a promising solid electrolyte for all-solid-state lithium-ion batteries (ASSLIBs), and its total conductivity is dramatically influenced by the ceramic microstructure. Here we report a novel aerodynamic levitation rapid solidification method to prepare dense LLTO ceramics with a dendrite-like microstructure, which can be hardly obtained by conventional sintering. At optimal nominal lithium content and cooling rate, the solidified LLTO ceramic achieved a high total conductivity of 2.5 × 10⁻⁴ S·cm⁻¹ at room temperature, along with excellent mechanical properties such as a high Young’s modulus of 240 GPa and a high hardness of 16.7 GPa. Results from this work suggest that aerodynamic levitation rapid solidification is an effective processing method to manipulate the microstructure of LLTO ceramics to minimize the GBs’ contribution to the total conductivity, which may be expanded to prepare other oxide-type lithium electrolytes. Full article

Janus hydrogels, defined by their asymmetric architectures and bifunctional interfaces, have emerged as a transformative class of solid-state electrolytes in electrochemical energy storage. By integrating spatially distinct chemomechanical and ionic functionalities within a single matrix, they overcome the intrinsic limitations of conventional isotropic hydrogels, offering enhanced interfacial stability, directional ion transport, and dendrite suppression in lithium- and zinc-based batteries. This mini-review systematically highlights recent breakthroughs in Janus hydrogel design, including interfacial polymerization and layer-by-layer assembly, which collectively enable precise modulation of crosslinking gradients and ion transport pathways. This review uniquely frames Janus hydrogels from a battery-centric and interface-engineering perspective. It elucidates key structure–function correlations, identifies current limitations in scalable fabrication and electrochemical longevity, and outlines future directions toward intelligent, multifunctional platforms for next-generation flexible and biointegrated energy systems. Full article

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

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

The increasing demand for safe, cost-effective, and sustainable energy storage solutions has spotlighted aqueous zinc-ion batteries (AZIBs) as promising alternatives to lithium-ion systems. However, the practical deployment of AZIBs remains hindered by dendritic growth, hydrogen evolution, and surface corrosion at the zinc metal anode, which severely compromise electrochemical stability. In this study, we propose an interfacial engineering strategy involving ultrathin diamond-like carbon (DLC) coatings applied to Zn anodes. The DLC films serve as conformal, ion-permeable barriers that mitigate parasitic side reactions and facilitate uniform Zn plating/stripping behavior. Materials characterizations of the DLC layer on the Zn anodes revealed the tunability of sp²/sp³ hybridization and surface morphology depending on DLC thickness. Electrochemical impedance spectroscopy demonstrated a significant reduction in interfacial resistance, particularly in the optimally coated sample (DLC2, ~20 nm), which achieved a favorable balance between mechanical integrity and ionic transport. Symmetric-cell tests confirmed enhanced cycling stability over 160 h, while full-cell configurations with an ammonium vanadate nanofiber-based cathode exhibited superior capacity retention over 900 cycles at 2 A g⁻¹. The DLC2-coated Zn anodes demonstrated the most effective performance, attributable to its moderate surface roughness, reduced disorder, and minimized charge-transfer resistance. These results provide insight into the importance of fine-tuning the DLC thickness and carbon bonding structure for suppressing dendrite formation and enhancing electrochemical stability. Full article

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

Sn-based anodes for lithium-ion batteries (LIBs) offer high capacity and low cost; however, significant volume changes during lithiation/delithiation cause mechanical degradation, limiting their practical applications. Microstructural control is a key approach to mitigating these volume changes. This study reports the fabrication of core (Sn rod)-shell (mesoporous Sn-oxide layer) structures through electrodeposition followed by anodization, and their applications to anode active materials for LIBs. First, micro-Sn rods with controlled lengths and diameters were fabricated under various electrodeposition conditions. The electrodeposited Sn exhibited a dendritic structure with short secondary rods branching from a long primary rod. While the primary Sn rod diameters remained constant, the secondary rod diameters varied depending on electrodeposition parameters. Notably, rod coarsening due to secondary rod agglomeration occurred at higher currents and longer deposition durations during galvanostatic electrodeposition. In contrast, potentiostatic electrodeposition prevented agglomeration and increased the quantity of Sn rods with voltage. Subsequently, the core-shell structures were fabricated by anodizing Sn rods, forming mesoporous Sn-oxide layers with different pore sizes and pore wall thicknesses. Electrochemical characterization revealed that the core-shell anode performance for LIBs varied with the Sn-oxide shell’s microstructure. These findings provide insights into optimal core-shell structures to improve anode performance for LIBs. Full article

Ultrafast-charging (UFC) technology for electric vehicles (EVs) and energy storage devices has brought with it an increase in demand for lithium-ion batteries (LIBs). However, although they pose advantages in driving range and charging time, LIBs face several challenges such as mechanical degradation, lithium dendrite formation, electrolyte decomposition, and concerns about thermal runaway safety. This review evaluates the key challenges and advances in LIB components (anodes, cathodes, electrolytes, separators, and binders), alongside innovations in charging protocols and safety concerns. Material-level solutions such as nanostructuring, doping, and composite architectures are investigated to improve ion diffusion, conductivity, and electrode stability. Electrolyte modifications, separator enhancements, and binder optimizations are discussed in terms of their roles in reducing high-rate degradation. Furthermore, charging protocols are addressed; adjustments can reduce mechanical and electrochemical stress on LIBs, decreasing capacity fade while providing rapid charging. This review highlights the key technological advancements that are enabling ultrafast charging and that are assisting us in overcoming severe limitations, paving the way for the development of next-generation high-performance LIBs. Full article

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

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

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

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