Search Results (343)

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

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

Polyethylene oxide (PEO) is the most well-studied polymer used in solid polymer electrolytes (SPEs) for lithium ion batteries (Li-ion batteries). However, ionic conductivity is greatly reduced in the low temperature range due to the crystallization of PEO. Therefore, methods to suppress the crystallization of PEO at room temperature by cross-linking or introducing a branched structure are currently being investigated. In this study, we synthesized new comb-type ion-conducting polyethers with two different side chains such as polydimethylsiloxane (PDMS) and polyethylene glycol monomethyl ether (mPEG) segments as flexible and ion-conducting segments, respectively. The introduction of the PDMS segment was found to prevent a decrease in ionic conductivity in the low-temperature region, but led to an ionic conductivity decrease in the high temperature region. On the other hand, the introduction of mPEG segments improved ionic conductivity in the high-temperature region. The introduction of mPEG segments with longer chains resulted in a significant decrease in ionic conductivity in the low-temperature region. Full article

Solid-state electrolytes (SSEs) have emerged as a promising solution for next-generation lithium-ion batteries due to their excellent safety and high energy density. However, their practical application is still hindered by critical challenges such as their low ionic conductivity and high interfacial resistance at room temperature. The innovative application of 3D printing in the field of electrochemistry, particularly in solid-state electrolytes, endows energy storage devices with attractive characteristics. In this study, ceramic-in-gel polymer electrolytes (GPEs) based on PVDF-HFP/PAN@LLZTO were fabricated using a direct ink writing (DIW) 3D printing technique. Under the optimal printing conditions (printing speed of 40 mm/s and fill density of 70%), the printed electrolyte exhibited a uniform and dense sponge-like porous structure, achieving a high ionic conductivity of 5.77 × 10⁻⁴ S·cm⁻¹, which effectively facilitated lithium-ion transport. A structural analysis indicated that the LLZTO fillers were uniformly dispersed within the polymer matrix, significantly enhancing the electrochemical stability of the electrolyte. When applied in a LiFePO₄|GPEs|Li cell configuration, the electrolyte delivered excellent electrochemical performance, with high initial discharge capacities of 168 mAh·g⁻¹ at 0.1 C and 166 mAh·g⁻¹ at 0.2 C, and retained 92.8% of its capacity after 100 cycles at 0.2 C. This work demonstrates the great potential of 3D printing technology in fabricating high-performance GPEs. It provides a novel strategy for the structural design and industrial scalability of lithium-ion batteries. Full article

Silicon-based anodes have emerged as promising candidates for advanced lithium-ion batteries (LIBs) owing to their outstanding lithium storage capacity; however, the commercial implementation of silicon-based anodes is hindered primarily by their significant volumetric changes and the resulting solid electrolyte interphase (SEI) instability during the lithiation/delithiation process. To overcome these issues, electrolyte optimization, particularly through the use of functional additives and solid-state electrolytes, has attracted significant research attention. In this paper, we review the recent developments in electrolyte additives, such as vinylene carbonate, fluoroethylene carbonate, and silane-based additives, and new additives, such as dimethylacetamide, that improve the SEI stability and overall electrochemical performance of silicon-based anodes. We also discuss the role of solid electrolytes, including oxides, sulfides, and polymer-based systems, in mitigating the volume changes in Si and improving safety. Such approaches can effectively enhance both the longevity and capacity retention of silicon-based anodes. Despite significant progress, further studies are essential to optimize electrolyte formulation and solve interfacial problems. Integrating these advances with improved electrode designs and anode materials is critical for realizing the full potential of silicon-based anodes in high-performance LIBs, particularly in electric vehicles and portable electronics. Full article

Solid polymer electrolytes (SPEs) have garnered significant attention due to their potential in all-solid-state batteries (ASSBs). However, adoption remains constrained by challenges such as low thermal stability and limited ionic conductivity. Here, we report on an electrospun (PAN/PEO)- conductive salt (LiBF₄) system, where the influence of varying polyacrylonitrile (PAN) and polyethylene oxide (PEO) ratios, along with different plasticizer concentrations, is evaluated. Notably, the 50:50 PAN/PEO sample exhibited the highest ionic conductivity, reaching 1∙10⁻² S/cm at 55 °C. This system also balanced conductivity and processability. Succinonitrile (SN) significantly influenced the morphology and conductivity. Samples with increased SN content showed enhanced capacity in symmetrical cells, achieving ~140 mAs/cm² for an 18:9:1 polymer (PAN/PEO):SN:conductive salt (LiBF₄) composition. The enhanced lithium-ion conductivity of the electrospun blend is attributed to the deliberate use of an unmixable PAN–PEO system. Their immiscibility creates well-defined interfacial regions within fibers, acting as efficient lithium-ion pathways. These findings support electrospun polymer blends as promising candidates for high-performance SPEs for ASSB development. Full article

Separators are generally considered inert components in lithium-ion batteries. In the past, some electroactive polymers have been successfully applied in separator modifications for overcharge protection or as acid scavengers. This study highlights the first use of two “electroactive” carbazole polymers (copolymer 9-phenyl-9H-carbazole-phenyl [PCP] and poly(9-vinylcarbazole) [PVC]), which were each applied separately as coatings on the cathode-facing side of commercial Celgard 2325 separators, respectively, to enhance the cycling performance of 0.3Li₂MnO₃·0.7LiMn_0.5Ni_0.5O₂//graphite (LMR-NM//Gr) full cells through interphase engineering. The team observed an irreversible polymer oxidation process of the carbazole-functionalized polymers—occurring only during the first charge—for the modified separator cells, and the results were confirmed by dQ/dV analysis, cyclic voltammetry measurements, and nuclear magnetic resonance characterizations. During this oxidation, carbazole polymers participate in the process of interphase formation, contributing to the improved cycling performance of LMR-NM//Gr batteries. Particularly, oxidation takes place at voltages of ~4.0 and ~3.5 V when PCP and PVC are used as separator coatings, which is highly irreversible. Further postmortem examinations suggest that the improvements using these modified separators arise from the formation of higher-quality and more inorganic SEI, as well as the beneficial CEI enriched in LixPOyFz. These interphases effectively inhibit the crosstalk effect by reducing TM dissolution. Full article

Batteries are used as energy storage devices in various equipment. Today, research is focused on solid-state batteries (SSBs), replacing the liquid electrolyte with a solid separator. The solid separators provide electrolyte stability, no leakage, and provide mechanical strength to the battery. Separators are mostly manufactured by either traditional processes or 3D printing technologies. These processes involve making a slurry of plastic, active and conductive material and usually adding a plasticizer when making thin films or filaments for 3D printing. This study investigates the additive manufacturing of solid-state electrolytes (SSEs) by employing fused deposition modeling (FDM) with recyclable, bio-derived polylactic acid (PLA) filaments. Precise control of macro-porosity is achieved by systematically varying key process parameters, including raster orientation, infill percentage, and interlayer adhesion conditions, thereby enabling the formation of tunable, interconnected pore networks within the polymer matrix. Following 3D printing, these engineered porous frameworks are infiltrated with lithium hexafluorophosphate (LiPF₆), which functions as the active ionic conductor. A tailored thermal sintering protocol is then applied to promote solid-phase fusion of the embedded salt throughout the macro-porous PLA scaffold, resulting in a mechanically robust and ionically conductive composite separator. The electrochemical ionic conductivity and structural integrity of the sintered SSEs are characterized through electrochemical impedance spectroscopy (EIS) and standardized mechanical testing to assess their suitability for integration into advanced solid-state battery architectures. The solid-state separator achieved an average ionic conductivity of 2.529 × 10⁻⁵ S·cm⁻¹. The integrated FDM-sintering process enhances ion exchange at the electrode–electrolyte interface, minimizes material waste, and supports cost-efficient, fully recyclable component fabrication. Full article

In polymer-based lithium batteries, polymer electrolytes (PEs) exhibit limited ionic conductivity at room temperature (25 °C). To address this issue, this paper describes a hexagonal-structure-based single-ion conducting gel polymer electrolyte (h-SICGPE) framework with a robust and efficient cross-linked polymer network, applicable to polymer-based batteries even at 25 °C. The proposed cross-linked polymer network backbone of the h-SICGPE, as a semisolid-state thin film type, has the homogeneous honeycomb structure incorporating anion receptor(s) inside each of its hexagonal closed cells and is obtained by cross-linking between trimethylolpropane tris(3-mercaptopropionate) and poly(ethylene glycol) diacrylate in a newly synthesized anion–receptor solution. The excellent structural capability of the h-SICGPE incorporating Li⁺/TFSI⁻ can enhance ionic conductivity and electrochemical stability by suppressing crystallinity and expanding free volume. Further, the anion receptor in its free volume helps to effectively increase the lithium-ion transference number by immobilizing counter-anions. Experimental results demonstrate dramatically superior performance at 25 °C, such as ionic conductivity (2.46 mS cm⁻¹), oxidative stability (4.9 V vs. Li/Li⁺), coulombic efficiency (97.65%), and capacity retention (88.3%). These results confirm the developed h-SICGPE as a promising polymer electrolyte for high-performance polymer-based lithium batteries operable at 25 °C. Full article

Due to their high energy density and power potential, 21700 lithium-ion battery cells are a widely used technology in hybrid and electric vehicles. Efficient thermal management is essential for maximizing the performance and capacity of Li-ion cells in both low- and high-temperature operating conditions. Optimizing thermal management systems remains critical, particularly for long-range and weight-sensitive applications. In these contexts, passive heat dissipation emerges as an ideal solution, offering effective thermal regulation with minimal additional system weight. This study aims to deepen the understanding of passive heat dissipation in 21700 battery cells and optimize their performance. Special emphasis is placed on analyzing heat transfer and the relative contributions of convective and radiative mechanisms under varying temperature and discharge conditions. Laboratory experiments were conducted under controlled environmental conditions at various discharge rates, ranging from 0.5×C to 5×C. A 3D-printed polymer casing was applied to the cell to enhance thermal dissipation, designed specifically to increase radiative heat transfer while minimizing system weight and reliance on active cooling solutions. Additionally, a numerical model was developed and optimized using experimental data. This model simulates convective and radiative heat transfer mechanisms with minimal computational demand. The optimized numerical model is intended to facilitate further investigation of the cell envelope strategy at the module and battery pack levels in future studies. Full article

To improve solid-state lithium batteries, solution casting has been employed to create lithium ion-conducting copolymer electrolytes involving poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/polyvinylpyrrolidone (PVP) blend polymers with various compositions. Following X-ray diffraction and Fourier transformation (FTIR), the structural characterisation and identification of molecular bonding in polymer electrolytes were confirmed. Through AC impedance analysis, the electrical characteristics of the solid-state polymer films were investigated. The dielectric conductivity of the sample was found to obey the modified Arrhenius relationship, while in the case of a sample with higher conductivity, it followed Arrhenius behaviour. The relaxation parameters and dielectric behaviour of the samples are demonstrated and discussed. Full article

In this study, the lithium-ion (Li-ion) battery type, which has a high-power density and utilizes lithium as the primary conductive terminal, has been employed. Within the scope of this research, a one-dimensional isothermal Li-ion battery model has been investigated under various electrolyte (both liquid and solid) and electrode materials using the COMSOL Multiphysics software. The obtained simulation results have been corroborated with information sourced from the literature and establish a foundational framework for future studies. The average range of electrolyte salt concentration in battery components is slightly higher for batteries utilizing polymer electrolytes compared to those with liquid electrolytes. During discharge at five different C-rates, Li-ion batteries with liquid electrolytes displayed higher voltage than those with polymer electrolytes. On the other hand, the one with the lithium iron phosphate (LFP) positive electrode exhibits the greatest variation in lithium concentration at the surface of the positive electrode at the end of discharge. Conversely, the battery using a LiNiO₂ cathode shows the smallest surface lithium concentration variation during the same period. This pattern is similarly observed for the lithium concentration at the center of the electrode particles. The presented model can be used to explore innovative electrolyte and electrode materials to improve the design of Li-ion batteries. Full article

The development of polymer binders with tailored functionalities and green manufacturing processes is highly needed for high-performance lithium–sulfur batteries. In this study, a readily hydrolyzable 3,9-divinyl-2,4,8,10-tetraoxaspiro-[5.5]-undecane is utilized to prepare a water-based binder. Specifically, the acrolein produced by hydrolysis undergoes in situ polymerization to form a linear polymer, while the other hydrolyzed product, pentaerythritol, physically crosslinks these polymer chains via hydrogen bonding, generating a network polymer (BTU). Additionally, gallic acid (GA), a substance derived from waste wood, is further introduced into BTU during slurry preparation, forming a biphenol-containing binder (BG) with a multi-hydrogen-bonded structure. This resilience and robust cathode framework effectively accommodate volumetric changes during cycling while maintaining efficient ion and electron transport pathways. Furthermore, the abundant polar groups in BG enable strong polysulfide adsorption. As a result, sulfur cathode with a high mass loading of 5.3 mg cm⁻² employing the BG (7:3) binder still retains an areal capacity of 4.7 mA h cm⁻² after 50 cycles at 0.1 C. This work presents a sustainable strategy for battery manufacturing by integrating renewable biomass-derived materials and eco-friendly aqueous processing to develop polymer binders, offering a green pathway to high-performance lithium–sulfur batteries. Full article

Polymer electrolytes (PEs) provide enhanced safety for high–energy–density lithium metal batteries (LMBs), yet their practical application is hampered by intrinsically low ionic conductivity and insufficient electrochemical stability, primarily stemming from suboptimal Li⁺ solvation environments and transport pathways coupled with slow polymer dynamics. Herein, we demonstrate a molecular design strategy to overcome these limitations by regulating the Li⁺ solvation structure through the synergistic interplay of conventional Lewis acid–base coordination and engineered hydrogen bond (H–bond) networks, achieved by incorporating specific H–bond donor functionalities (N,N′–methylenebis(acrylamide), MBA) into the polymer architecture. Computational modeling confirms that the introduced H–bonds effectively modulate the Li⁺ coordination environment, promote salt dissociation, and create favorable pathways for faster ion transport decoupled from polymer chain motion. Experimentally, the resultant polymer electrolyte (MFE, based on MBA) enables exceptionally stable Li metal cycling in symmetric cells (>4000 h at 0.1 mA cm⁻²), endows LFP|MFE|Li cells with long–term stability, achieving 81.0% capacity retention after 1400 cycles, and confers NCM622|MFE|Li cells with cycling endurance, maintaining 81.0% capacity retention after 800 cycles under a high voltage of 4.3 V at room temperature. This study underscores a potent molecular engineering strategy, leveraging synergistic hydrogen bonding and Lewis acid–base interactions to rationally tailor the Li⁺ solvation structure and unlock efficient ion transport in polymer electrolytes, paving a promising path towards high–performance solid–state lithium metal batteries. Full article

Lithium-ion batteries are restricted in development due to safety issues such as poor chemical stability and flammability of organic liquid electrolytes. Replacing liquid electrolytes with solid ones is crucial for improving battery safety and performance. This study aims to enhance the performance of polyethylene oxide (PEO)-based polymer via blending with poly(vinylidene fluoride-hexafluoropropylene) (P(VDF-HFP)). The experimental results showed that the addition of P(VDF-HFP) disrupted the crystalline regions of PEO by increasing the amorphous domains, thus improving lithium-ion migration capability. The electrolyte membrane with 30 wt% P(VDF-HFP) and 70 wt% PEO exhibited the highest ionic conductivity, widest electrochemical window, and enhanced thermal stability, as well as a high lithium-ion transference number (0.45). The cells assembled with this membrane electrolyte demonstrated an excellent rate of performance and cycling stability, retaining specific capacities of 122.39 mAh g⁻¹ after 200 cycles at 0.5C, and 112.77 mAh g⁻¹ after 200 cycles at 1C and 25 °C. The full cell assembled with LiFePO₄ as the positive electrode exhibits excellent rate performance and good cycling stability, indicating that prepared solid electrolytes have great potential applications in lithium batteries. Full article