Search Results (110)

This study reports a graphite-core, multiphase gradient C–Si–N composite architecture for Si-containing graphite-based negative electrodes in lithium-ion batteries. The increase in electrode thickness is used as a practical metric of expansion-driven degradation. The composite is prepared by the simultaneous nitridation and carbonization of a graphite core–Si precursor using polyvinylpyrrolidone (PVP) as the N source. Scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy indicates a quasi-continuous radial trend in the relative N signal toward the outer shell, consistent with preferential N enrichment near the particle exterior. This spatially distributed N arrangement may spatially separate the Si-rich expansion-prone region from the carbon-rich exterior containing nitrides and other N-bearing species, thereby enabling stress partitioning. The shell architecture is designed to disperse expansion-induced stress and stabilize the electrode–electrolyte interface. During electrochemical cycling, the C–Si–N electrode with 10% PVP preserves its core–shell morphology and exhibits the smallest average electrode thickness expansion (~58% after 40 cycles, based on four independent cells). The reduced thickness growth is discussed in relation to a mechanically robust Si–N matrix (Si₃N₄-like/SiN_x-like), potential Li–N interphase species, and N-containing carbon, together with the post-mortem morphology and electrochemical impedance evolution. This study presents reduced swelling as an electrode-level trend versus nominal PVP addition, along with associated nitride-related signatures, thereby highlighting spatially graded stress buffering as an electrode-level design principle. Full article

Silicon-based materials offer exceptional theoretical capacity for lithium-ion batteries (LIBs), but their practical application remains severely hindered by large volume expansion, low electrical conductivity, and unstable solid electrolyte interphase (SEI) formation during cycling. Herein, a binder-free silicon-containing carbon composite anode (denoted as CP-Si@C-4, where CP represents the conductive carbon paper substrate) is designed: carbon constitutes the structural and conductive framework, while silicon nanoparticles serve as a functional alloying component contributing characteristic lithiation/delithiation behavior. This framework comprises a conductive carbon paper (CP) scaffold, a resin-derived carbon matrix for homogeneous silicon dispersion, an interconnected carbon nanotube (CNT) network enabling long-range electron transport, and a conformal chemical vapor deposition (CVD) carbon layer for interfacial stabilization. Rather than simply increasing the overall carbon content, a series of control electrodes with distinct carbon configurations are deliberately designed to decouple the respective roles of bulk stress buffering and particle-level interfacial stabilization during cycling. The results indicate that functionally differentiating and coordinately regulating these two functions is critical for achieving durable binder-free silicon-containing carbon composite anodes. Benefiting from this cooperative multidimensional carbon architecture, the optimized CP-Si@C-4 anode delivers an initial Coulombic efficiency (ICE) of 86.3% and maintains a reversible capacity of ~990 mA h g⁻¹ at 2 A g⁻¹ after 1000 cycles. This work provides a structural design concept for improving long-term stability in binder-free silicon-containing carbon composite anodes. Full article

Silicon (Si) has attracted extensive attention as a promising anode material for next-generation lithium-ion batteries (LIBs) due to its ultra-high theoretical capacity, low lithiation potential, and economic advantages. However, drastic volume expansion during cycling and slow reaction kinetics severely compromise its structural stability and practical application. Recently, two-dimensional (2D) MXenes have been explored as effective functional components in Si-based electrodes because of their excellent electrical conductivity, high specific surface area, adjustable surface terminations, and mechanical robustness. When integrated with Si, MXenes serve as conductive matrices that alleviate volumetric stress, enhance charge transport, and accelerate electron/ion diffusion. Consequently, Si/MXene nanocomposites (NCs) exhibit significantly improved lithium (Li) storage performance. This review outlines recent advances in Si/MXene NCs, covering fabrication strategies, structural engineering, and various configurations, including particulate materials, three-dimensional (3D) architectures, films, and fibrous systems, and establishes the relationship between structural design and electrochemical behavior. Remaining challenges and prospective research directions are also discussed to guide the development of high-energy-density LIB anodes. Full article

The rapid increase in electric vehicle (EV) adoption necessitates advanced charging infrastructures that are compact, efficient, and capable of bidirectional power flow for both vehicle-to-grid (V2G) and grid-to-vehicle (G2V) operation. Unlike traditional silicon and SiC-based chargers, this work introduces a Ga₂O₃-based bidirectional smart charging system integrated with a hybrid energy storage system to deliver superior performance. A coordinated control strategy is developed to regulate power sharing between a supercapacitor and a lithium-ion battery pack, thereby extending battery life, reducing current stress, and providing effective transient support. This hybrid system employs PI-based control and advanced modulation techniques to minimize current ripple, maintain the unity power factor, and ensure stable DC-link voltage regulation. MATLAB/Simulink simulation results demonstrate robust DC-link stability, smooth bidirectional power transfer, and very low total harmonic distortion. Comparative loss analysis shows that Ga₂O₃ MOSFETs offer significantly lower conduction and switching losses, enabling efficiencies up to 98% across the rated operating range. These results confirm that the proposed charger is highly suitable for next-generation EV infrastructures requiring high power density, reliable grid interfacing, and enhanced operational longevity. A hardware prototype was also developed and tested, with experimental results validating reliable grid-side performance and efficient energy sharing under typical operating conditions. Full article

Silicon is a well-known anode material for lithium-ion batteries that has attracted a lot of interests because of its high theoretical specific capacity (4200 mAh g⁻¹). However, its severe volume expansion during cycling leads to structural degradation and rapid capacity fading. The design of porous silicon architectures has emerged as a fundamental and effective strategy to mitigate these issues by accommodating mechanical stress and preserving electrode integrity. Concurrently, the development of advanced in situ/operando characterization techniques has shifted the research paradigm, enabling direct observation of dynamic structural and interfacial evolution under operating conditions. This review systematically summarizes recent progress in the rational design of porous Si-based anodes and critically examines how state-of-the-art in situ methods provide direct mechanistic validation of these designs. The work highlights the synergistic interplay between targeted material engineering and in situ/operando characterization, offering a roadmap for the development of high-performance porous silicon anodes. Full article

Waterborne polyurethane (WPU) and waterborne poly(urethane-urea) (WPUU) dispersions allow safer and more sustainable manufacturing of rechargeable batteries via water-based processing, while offering tunable adhesion and segmented-domain mechanics. Beyond conventional roles as binders and coatings, WPU/WPUU chemistries also support separator/interlayer and polymer-electrolyte designs for lithium-ion and lithium metal systems, where interfacial integrity, stress accommodation, and ion transport must be balanced. Here, we review WPU/WPUU fundamentals (building blocks, dispersion stabilization, morphology, and film formation) and review prior studies through a battery-centric structure–processing–property lens. We point out key performance-limiting trade-offs—adhesion versus electrolyte uptake and ionic conductivity versus storage modulus—and relate them to practical formulation variables, including soft-/hard-segment selection, ionic center/counterion design, molecular weight/topology control, and crosslinking strategies. Applications are reviewed for (i) electrode binders (graphite/Si; cathodes such as LFP and NMC), (ii) separator coatings and functional interlayers, and (iii) gel/solid polymer electrolytes and hybrid composites, with a focus on practical design guidelines for navigating these trade-offs. Future advancements in WPU/WPUU chemistries will depend on developing stable, low-impedance interlayers, enhancing electrochemical behavior, and establishing application-specific design guidelines to optimize performance in lithium metal batteries (LMB). Full article

Silicon oxide/graphite (SiO_x/Gr) anodes are promising candidates for high energy-density lithium-ion batteries. However, their complex multiphysics degradation mechanisms pose challenges for accurately interpreting and predicting capacity fade behavior. In particular, existing multiphysics models typically treat gas generation and solid electrolyte interphase (SEI) growth as independent or unidirectionally coupled processes, neglecting their bidirectional interactions. Here, we develop an electro–thermal–mechanical–gaseous coupled model to capture the dominant degradation processes in SiO_x/Gr anodes, including SEI growth, gas generation, SEI formation on cracks, and particle fracture. Model validation shows that the proposed framework can accurately reproduce voltage responses under various currents and temperatures, as well as capacity fade under different thermal and mechanical conditions. Based on this validated model, a mechanistic analysis reveals two key findings: (1) Gas generation and SEI growth are bidirectionally coupled. SEI growth induces gas release, while accumulated gas in turn regulates subsequent SEI evolution by promoting SEI formation through hindered mass transfer and suppressing it through reduced active surface area. (2) Crack propagation within particles is jointly governed by the magnitude and duration of stress. High-rate discharges produce large but transient stresses that restrict crack growth, while prolonged stresses at low rates promote crack propagation and more severe structural degradation. This study provides new insights into the coupled degradation mechanisms of SiO_x/Gr anodes, offering guidance for performance optimization and structural design to extend battery cycle life. Full article

This study aims to fabricate magnesium-doped SiOx materials through the integrated application of physical vapor deposition and chemical vapor deposition techniques, with the objective of developing high-performance anode materials for lithium-ion batteries. With the macroscopic particle size held constant, this study endeavors to explore the impact of variations in the size of microscopic silicon crystals on the properties of the material. Under the effect of magnesium doping, the influence mechanism of different microscopic grain sizes on the reaction kinetics behavior and structural stability of the material was systematically studied. Based on the research findings, a reasonable control range for the size of silicon crystals will be proposed. The research findings indicate that both relatively small and large silicon crystals are disadvantageous for cycling performance. When the silicon crystal grain size is 5.79 nm, the composite material demonstrates a relatively high overall capacity of 1442 mAh/g and excellent cycling stability. After 100 cycles, the capacity retention rate reaches 83.82%. EIS analysis reveals that larger silicon crystals exhibit a higher lithium ion diffusion coefficient. As a result, the silicon electrodes show more remarkable rate performance. Even under a high current density of 1C, the capacity of the material can still be maintained at 1044 mAh/g. Full article

Silicon-graphite anodes offer a practical route to increase the energy density of lithium-ion batteries (LIBs), but their widespread adoption is hampered by cyclic instability due to huge volume changes of silicon during lithiation/delithiation process. Another fallout of LIBs capacity gain is growing safety concerns due to fire risks, associated with the uncontrolled release of chemical energy. Herein, we test a hexakis(fluoroethoxy)phosphazene (HFEPN) as a multifunctional electrolyte additive designed to mitigate both issues. The flammability of HFEPN-containing electrolytes was evaluated using a self-extinguishing time test, while the electrochemical performance was assessed in Si/C composite||NMC pouch cells under a progressively accelerated cycling protocol. It is shown that the additive fully imparts flame-retardant properties to the electrolyte at a 15 wt% loading. Despite forming a more stable solid–electrolyte interphase (SEI) with enhanced interfacial kinetics the additive did not improve the cycling stability of the Si/C-based cells. The cells with 15 wt% HFEPN retained 43% of capacity after 70 cycles, comparable to 46.5% for the reference electrolyte. The diffusion limitations imposed by the increased electrolyte viscosity are assumed to offset the interfacial benefits of the additive. Thus, alongside the improved synthetic route, this study demonstrates that while HFEPN functions as an effective flame retardant and SEI modifier, its practical benefits for silicon anodes are limited at high concentrations by detrimental effects on electrolyte transport properties and should be improved in future molecular design efforts. Full article

While we are pursuing a fully electrified society, high-energy rechargeable batteries are undergoing intensive investigation. In this respect, atomic and molecular layer deposition (ALD and MLD) have been drawing increasing interest, due to their unmatched capabilities to precisely modify electrodes’ surfaces for better electrochemical performance. In this work, we reviewed the recent studies using ALD/MLD for interface engineering of several important electrode materials, including nickel (Ni)-rich metal oxide cathodes, silicon (Si), and lithium (Li) anodes in lithium-ion and lithium metal batteries. We particularly discussed the most promising coatings from these studies and explored the underlying mechanisms based on experiments and modeling. We anticipate that this work will inspire more studies using ALD/MLD as an important technique for securing new solutions for batteries. Full article

Enhancing the safety of lithium-ion batteries (LIBs) by replacing flammable electrolytes is a key challenge. Ionic liquid (IL)-based electrolytes are considered an interesting alternative due to their thermal and chemical stability, high voltage stability window, and tunable properties. This study investigates the electrochemical behavior of two newly synthesized ILs, comparing them to conventional alkyl carbonate-based electrolytes. Nitrogen-doped carbon silicon oxycarbide (NC-SiOC), used as the active material in negative electrodes, was combined with two polymeric binders: poly(acrylic acid) (PAA) and poly(acrylonitrile) (PAN). NC-SiOC/PAN electrodes exhibited a significantly higher initial charge capacity—approximately 25–30% greater than their PAA-based counterparts in the first cycle at 0.1 A g⁻¹ (850–990 mAh g⁻¹ vs. 600–700 mAh g⁻¹), and demonstrated an improved initial Coulombic efficiency (67% vs. 62%). Long-term cycling stability over 1000 cycles at 1.6 A g⁻¹ retained 75–80% of the initial 0.1 A g⁻¹ capacity. This outstanding performance is attributed to the synergistic effects of nitrogen-rich carbonaceous phases within the NC-SiOC material and the cyclized-PAN binder, which facilitate structural stability by accommodating volumetric changes and enhancing solid electrolyte interphase (SEI) stability. Notably, despite the lower ionic transport properties of the IL electrolytes, their incorporation did not compromise performance, supporting their feasibility as safer electrolyte alternatives. These findings offer one of the most promising electrochemical performances reported for SiOC materials to date. Full article

Lithium-ion batteries (LIBs) have become the dominant energy storage technology due to their versatility and superior performance across diverse applications. Silicon (Si) stands out as a particularly promising high-capacity anode material for next-generation LIBs, offering a theoretical capacity nearly ten times greater than conventional graphite anodes. However, its practical implementation faces a critical challenge: the material undergoes a ~300% volume expansion during lithiation/delithiation, which causes severe mechanical stress, electrode pulverization, and rapid capacity decay. In addressing these limitations, advanced polymer binders serve as essential components for preserving the structural integrity of Si-based anodes. Notably, self-healing polymeric binders have emerged as a groundbreaking solution, capable of autonomously repairing cycle-induced damage and significantly enhancing electrode durability. The evaluation of self-healing performance is generally based on mechanical characterization methods while morphological observations by scanning electron microscopy provide direct evidence of crack closure; for electrochemically active materials, electrochemical techniques including GCD, EIS, and CV are employed to monitor recovery of functionality. In this study, a novel self-healing copolymer (PHX-23) was synthesized for Si anodes using a combination of octadecyl acrylate (ODA), methacrylic acid (MA), 2-hydroxyethyl methacrylate (HEMA), and polyethylene glycol methyl ether methacrylate (PEGMA). The copolymer was thoroughly characterized using NMR, FTIR, TGA, SEM, and EDX to confirm its chemical structure, thermal stability, and morphology. Electrochemical evaluation revealed that the PHX-23 binder markedly improves cycling stability, sustaining a reversible capacity of 427 mAh g⁻¹ after 1000 cycles at 1C. During long-term cycling, the Coulombic efficiency of the PHX-23 polymer is 99.7%, and similar functional binders in the literature have shown similar results at lower C-rates. Comparative analysis with conventional binders (e.g., PVDF and CMC/SBR) demonstrated PHX-23’s exceptional performance, exhibiting higher capacity retention and improved rate capability. These results position PHX-23 as a transformative binder for silicon anodes in next-generation lithium-ion batteries. Full article

The application of silicon–carbon (Si/C) composite materials in lithium-ion batteries faces problems regarding volume expansion and surface defects. Although coating is a popular modification scheme in the market, the influence of carbon layer quality on the electrochemical performance of Si/C still needs to be studied. By comparing the carbon layers produced by solid-phase and liquid-phase coating methods, an innovative solid–liquid coating technology was proposed to prepare high-strength and high-stiffness carbon layers, and the effects of different coating processes on the physical, mechanical, and electrochemical properties of the materials were systematically studied. Through physical properties and electrochemical testing, it was found that the solid–liquid coating method (Si/C@Pitch+RGFQ) can form a carbon layer with the least defects and the highest density. Compared with solid-phase coating and liquid-phase coating, its specific surface area (SSA) and carbon increment are the lowest, and the surface carbon content and oxygen content are significantly reduced after solid–liquid coating. Mechanical performance tests show that the Young’s modulus of the carbon layer prepared by this method reaches 30.3 GPa, demonstrating excellent structural strength and elastic deformation ability. The first coulombic efficiency (ICE) of Si/C@Pitch+RGFQ reached 88.17%, the interface impedance (23.2 Ω) was the lowest, and the lithium-ion diffusion coefficient was significantly improved. At a rate of 0.1 C to 2 C, the capacity retention rate is excellent. After one hundred and a half-cell cycles, the remaining capacity is 1420.5 mAh/g, and the capacity retention rate reaches 92.4%. The full-cell test further proves that the material has a capacity retention rate of 82.3% and 81.3% after 1000 cycles at room temperature and high temperature (45 °C), respectively. At the same time, it has good rate performance and high-/low-temperature performance, demonstrating good commercial application potential. The research results provide a key basis for the optimized preparation of the surface carbon layer of Si/C composite materials and promote the practical application of high-performance silicon-based negative electrode materials. Full article

Silicon carbide (SiC) and silicon nanoparticle-decorated carbon (Si/C) materials are electrodes that can potentially be used in various rechargeable batteries, owing to their inimitable merits, including non-flammability, stability, eco-friendly nature, low cost, outstanding theoretical capacity, and earth abundance. However, SiC has inferior electrical conductivity, volume expansion, a low Li⁺ diffusion rate during charge–discharge, and inevitable repeated formation of a solid–electrolyte interface layer, which hinders its commercial utilization. To address these issues, extensive research has focused on optimizing preparation methods, engineering morphology, doping, and creating composites with other additives (such as carbon materials, metal oxides, nitrides, chalcogenides, polymers, and alloys). Owing to the upsurge in this research arena, providing timely updates on the use of SiC and Si/C for batteries is of great importance. This review summarizes the controlled design of SiC-based and Si/C composites using various methods for rechargeable metal-ion batteries like lithium-ion (LIBs), sodium-ion (SIBs), zinc-air (ZnBs), and potassium-ion batteries (PIBs). The experimental and predicted theoretical performance of SiC composites that incorporate various carbon materials, nanocrystals, and non-metal dopants are summarized. In addition, a brief synopsis of the current challenges and prospects is provided to highlight potential research directions for SiC composites in batteries. Full article

In most commercial lithium-ion batteries, graphite remains the primary anode material. However, its theoretical specific capacity is only 372 mAh∙g⁻¹, which falls short of meeting the demands of high-performance electronic devices. Silicon anodes, despite boasting an ultra-high theoretical specific capacity of 4200 mAh∙g⁻¹, suffer from significant volume expansion (>300%) during cycling, leading to severe capacity fade and limiting their commercial viability. Currently, silicon-based polymer-derived ceramics have emerged as a highly promising next-generation anode material for lithium-ion batteries, thanks to their unique nano-cluster structure, tunable composition, and low volume expansion characteristics. The maximum capacity of the ceramics can exceed 1000 mAh∙g⁻¹, and their unique synthesis routes enable customization to align with diverse electrochemical application requirements. In this paper, we present the progress of silicon oxycarbide (SiOC), silicon carbonitride (SiCN), silicon boron carbonitride (SiBCN) and silicon oxycarbonitride (SiOCN) in the field of LIBs, including their synthesis, structural characteristics and electrochemical properties, etc. The mechanisms of lithium-ion storage in the Si-based anode materials are summarized as well, including the key role of free carbon in these materials. Full article