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Search Results (1,388)

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27 pages, 8108 KB  
Review
A Review of Cross-Scale State Estimation Techniques for Power Batteries in Electric Vehicles: Evolution from Single-State to Multi-State Cooperative Estimation
by Ning Chen, Yihang Xie, Yuanhao Cheng, Huaiqing Wang, Yu Zhou, Xu Zhao, Jiayao Chen and Chunhua Yang
Energies 2025, 18(19), 5289; https://doi.org/10.3390/en18195289 - 6 Oct 2025
Abstract
As a critical technological foundation for electric vehicles, power battery state estimation primarily involves estimating the State of Charge (SOC), the State of Health (SOH) and the Remaining Useful Life (RUL). This paper systematically categorizes battery state estimation methods into three distinct generations, [...] Read more.
As a critical technological foundation for electric vehicles, power battery state estimation primarily involves estimating the State of Charge (SOC), the State of Health (SOH) and the Remaining Useful Life (RUL). This paper systematically categorizes battery state estimation methods into three distinct generations, tracing the evolutionary progression from single-state to multi-state cooperative estimation approaches. First-generation methods based on equivalent circuit models offer straightforward implementation but accumulate SOC-SOH estimation errors during battery aging, as they fail to account for the evolution of microscopic parameters such as solid electrolyte interphase film growth, lithium inventory loss, and electrode degradation. Second-generation data-driven approaches, which leverage big data and deep learning, can effectively model highly nonlinear relationships between measurements and battery states. However, they often suffer from poor physical interpretability and generalizability due to the “black-box” nature of deep learning. The emerging third-generation technology establishes transmission mechanisms from microscopic electrode interface parameters via electrochemical impedance spectroscopy to macroscopic SOC, SOH, and RUL states, forming a bidirectional closed-loop system integrating estimation, prediction, and optimization that demonstrates potential to enhance both full-operating-condition adaptability and estimation accuracy. This progress supports the development of high-reliability, long-lifetime electric vehicles. Full article
(This article belongs to the Section E: Electric Vehicles)
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16 pages, 4514 KB  
Article
LATP-Enhanced Polymer Electrolyte for an Integrated Solid-State Battery
by Xianzheng Liu, Nashrah Hani Jamadon, Liancheng Zheng, Rongji Tang and Xiangjun Ren
Polymers 2025, 17(19), 2673; https://doi.org/10.3390/polym17192673 - 2 Oct 2025
Abstract
Traditional liquid electrolyte batteries face safety concerns such as leakage and flammability, while further optimization has reached a bottleneck. Solid electrolytes are therefore considered a promising solution. Here, a PEO–LiTFSI–LATP (PELT) composite electrolyte was developed by incorporating nanosized Li1.3Al0.3Ti [...] Read more.
Traditional liquid electrolyte batteries face safety concerns such as leakage and flammability, while further optimization has reached a bottleneck. Solid electrolytes are therefore considered a promising solution. Here, a PEO–LiTFSI–LATP (PELT) composite electrolyte was developed by incorporating nanosized Li1.3Al0.3Ti1.7(PO4)3 fillers into a polyethylene oxide matrix, effectively reducing crystallinity, enhancing mechanical robustness, and providing additional Li+ transport channels. The PELT electrolyte exhibited an electrochemical stability window of 4.9 V, an ionic conductivity of 1.2 × 10−4 S·cm−1 at 60 °C, and a Li+ transference number (tLi+) of 0.46, supporting stable Li plating/stripping for over 600 h in symmetric batteries. More importantly, to address poor electrode–electrolyte contact in conventional layered cells, we proposed an integrated electrode–electrolyte architecture by in situ coating the PELT precursor directly onto LiFePO4 cathodes. This design minimized interfacial impedance, improved ion transport, and enhanced electrochemical stability. The integrated PELT/LFP battery retained 74% of its capacity after 200 cycles at 1 A·g−1 and showed superior rate capability compared with sandwich-type batteries. These results highlight that coupling LATP-enhanced polymer electrolytes with an integrated architecture is a promising pathway toward high-safety, high-performance solid-state lithium-ion batteries. Full article
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13 pages, 1846 KB  
Article
Toward Circular Carbon: Upcycling Coke Oven Waste into Graphite Anodes for Lithium-Ion Batteries
by Seonhui Choi, Inchan Yang, Byeongheon Lee, Tae Hun Kim, Sei-Min Park and Jung-Chul An
Batteries 2025, 11(10), 365; https://doi.org/10.3390/batteries11100365 - 2 Oct 2025
Abstract
This study presents a sustainable upcycling strategy to convert “Pit,” a carbon-rich coke oven by-product from steel manufacturing, into high-purity graphite for use as an anode material in lithium-ion batteries. Despite its high carbon content, raw Pit contains significant impurities and has irregular [...] Read more.
This study presents a sustainable upcycling strategy to convert “Pit,” a carbon-rich coke oven by-product from steel manufacturing, into high-purity graphite for use as an anode material in lithium-ion batteries. Despite its high carbon content, raw Pit contains significant impurities and has irregular particle morphology, which limits its direct application in batteries. We employed a multi-step, additive-free refinement process—including jet milling, spheroidization, and high-temperature graphitization—to enhance carbon purity and structural properties. The processed Pit-derived graphite showed a much-improved particle size distribution (D50 reduced from 25.3 μm to 14.8 μm & Span reduced from 1.72 to 1.23), increased tap density (from 0.54 to 0.80 g/cm3), and reduced BET surface area, making it suitable for high-performance lithium-ion batteries anodes. Structural characterization by XRD and TEM confirmed dramatically enhanced crystallinity after graphitization (graphitization degree increasing from ~13 for raw Pit to 95.7% for graphitized Pit at 3000 °C). The fully processed graphite (denoted S_Pit3000) delivered a reversible discharge capacity of 346.7 mAh/g with an initial Coulombic efficiency of 93.5% in half-cell tests—comparable to commercial artificial graphite. Furthermore, when composited with silicon oxide to form a hybrid anode, the material achieved an even higher capacity of 418.0 mAh/g under high mass loading conditions. These results highlight the feasibility of transforming industrial coke waste into value-added electrode materials through environmentally friendly physical processes. The upcycled graphite anode meets industrial performance standards, demonstrating a promising route toward circular economy solutions in both the steel and battery industries. Full article
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13 pages, 2339 KB  
Article
Preparation of Silk Fibroin–Carboxymethyl Cellulose Composite Binder and Its Application in Silicon-Based Anode for Lithium-Ion Batteries
by Shuai Huang, Ruyi Wang, Mingke Lei, Qingxuan Geng, Qingwei Li, Jiwei Zhang and Jingwei Zhang
Nanomaterials 2025, 15(19), 1509; https://doi.org/10.3390/nano15191509 - 2 Oct 2025
Abstract
The molecular structure and mechanical resilience of the binder are crucial for mitigating volume expansion, maintaining electrode structural integrity, and enhancing the cycling stability of silicon-based anode materials in lithium-ion batteries. In this study, from the perspective of binder molecular structural design, commercial [...] Read more.
The molecular structure and mechanical resilience of the binder are crucial for mitigating volume expansion, maintaining electrode structural integrity, and enhancing the cycling stability of silicon-based anode materials in lithium-ion batteries. In this study, from the perspective of binder molecular structural design, commercial carboxymethyl cellulose (CMC) was modified with silk protein (SF), which has good mechanical properties and abundant surface functional groups, to address issues such as high brittleness, poor compliance and easy cracking of the electrode structure during charge and discharge cycles, and to enhance the mechanical properties of the CMC-based binder and its interaction with silicon particles, so as to improve the cycle stability of silicon-based materials. The mechanical properties of the CMC binder were significantly improved and the interaction between the binder and the surface of the silicon particles was enhanced by the addition of SF. When the SF content was optimized at 6 wt%, the electrode exhibited the best electrochemical performance, delivering a specific capacity of 1182 mAh/g at a high current density of 5000 mA/g, and retaining a capacity of 1138 mAh/g after 50 cycles at 1000 mA/g, demonstrating excellent electrochemical durability. Full article
(This article belongs to the Section Energy and Catalysis)
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12 pages, 2321 KB  
Communication
Intergranular Crack of Cathode Materials in Lithium-Ion Batteries Subjected to Rapid Cooling During Transient Thermal Runaway
by Siqi Li, Changchun Ye, Ming Jin, Guobin Zhong, Shi Liu, Yajie Liu and Zhixin Tai
Batteries 2025, 11(10), 363; https://doi.org/10.3390/batteries11100363 - 30 Sep 2025
Abstract
In metallurgy, the quenching process often induces changes in certain material properties, such as hardness and ductility, through the rapid cooling of a workpiece in water, gas, oil, polymer, air, or other fluids. Given that lithium-ion batteries operate under relatively benign conditions, conventional [...] Read more.
In metallurgy, the quenching process often induces changes in certain material properties, such as hardness and ductility, through the rapid cooling of a workpiece in water, gas, oil, polymer, air, or other fluids. Given that lithium-ion batteries operate under relatively benign conditions, conventional rapid cooling does not significantly affect the property variations in their internal electrode materials during normal use. However, thermal runaway presents an exception due to its dramatic temperature fluctuations from room temperature to several hundred degrees Celsius. In this study, we investigated NCM811 cathodes in 18,650 batteries subjected to transient thermal runaway followed by rapid cooling using several advanced analytical techniques. The results reveal a phenomenon characterized by intergranular cracking within NCM811 cathode materials when exposed to rapid cooling during transient thermal runaway. Furthermore, lithium-ion cells utilizing reused NCM-182.4 electrodes in fresh electrolyte demonstrate a reversible capacity of 231.4 mAh/g after 30 cycles at 0.1 C, highlighting the potential for reusing NCM811 cathodes in the lithium-ion battery recycling process. These findings not only illustrate that NCM811 particles may experience intergranular cracking when subjected to rapid cooling during transient thermal runaway, but also the rapidly cooled NCM811 electrodes exhibit potential for reuse. Full article
(This article belongs to the Special Issue Battery Interface: Analysis & Design)
16 pages, 2423 KB  
Article
Numerical Simulation Study and Stress Prediction of Lithium-Ion Batteries Based on an Electrochemical–Thermal–Mechanical Coupled Model
by Juanhua Cao and Yafang Zhang
Batteries 2025, 11(10), 360; https://doi.org/10.3390/batteries11100360 - 29 Sep 2025
Abstract
In lithium-ion batteries, the fracture of active particles that are under stress is a key cause of battery aging, which leads to a reduction in active materials, an increase in internal resistance, and a decay in battery capacity. A coupled electrochemical–thermal–mechanical model was [...] Read more.
In lithium-ion batteries, the fracture of active particles that are under stress is a key cause of battery aging, which leads to a reduction in active materials, an increase in internal resistance, and a decay in battery capacity. A coupled electrochemical–thermal–mechanical model was established to study the concentration and stress distributions of negative electrode particles under different charging rates and ambient temperatures. The results show that during charging, the maximum lithium-ion concentration occurs on the particle surface, while the minimum concentration appears at the particle center. Moreover, as the temperature decreases, the concentration distribution of negative electrode active particles becomes more uneven. Stress analysis indicates that when charging at a rate of 1C and 0 °C, the maximum stress of particles at the negative electrode–separator interface reaches 123.7 MPa, while when charging at 30 °C, the maximum particle stress is 24.3 MPa. The maximum shear stress occurs at the particle center, presenting a tensile stress state, while the minimum shear stress is located on the particle surface, showing a compressive stress state. Finally, to manage the stress of active materials in lithium-ion batteries while charging for health maintenance, this study uses a DNN (Deep Neural Network) to predict the maximum shear stress of particles based on simulation results. The predicted indicators, MAE (Mean Absolute Error) and RMSE (Root Mean Square Error), are 0.034 and 0.046, respectively. This research is helpful for optimizing charging strategies based on the stress of active materials in lithium-ion batteries during charging, inhibiting battery aging and improving safety performance. Full article
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36 pages, 3877 KB  
Review
Swelling Mechanisms, Diagnostic Applications, and Mitigation Strategies in Lithium-Ion Batteries
by Sahithi Maddipatla, Huzaifa Rauf, Michael Osterman, Naveed Arshad and Michael Pecht
Batteries 2025, 11(10), 356; https://doi.org/10.3390/batteries11100356 - 28 Sep 2025
Abstract
Electrochemical processes within a lithium-ion battery cause electrode expansion and gas generation, thus resulting in battery swelling and, in severe cases, reliability and safety issues. This paper presents the mechanisms responsible for swelling, including thermal expansion, lithium intercalation, electrode interphase layer growth, lithium [...] Read more.
Electrochemical processes within a lithium-ion battery cause electrode expansion and gas generation, thus resulting in battery swelling and, in severe cases, reliability and safety issues. This paper presents the mechanisms responsible for swelling, including thermal expansion, lithium intercalation, electrode interphase layer growth, lithium plating, and gas generation, while highlighting their dependence on material properties, design considerations, C-rate, temperature, state of charge (SoC), and voltage. The paper then discusses how swelling correlates with capacity fade, impedance rise, and thermal runaway, and demonstrates the potential of using swelling as a diagnostic and prognostic metric for battery health. Swelling models that connect microscopic mechanisms to macroscopic deformation are then presented. Finally, the paper presents strategies to mitigate swelling, including materials engineering, surface coatings, electrolyte formulation, and mechanical design modifications. Full article
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12 pages, 2405 KB  
Article
Impact of Inert Materials on Commercial Lithium–Ion Cell Energy Density
by William Yourey, Kayla Nong and Bhanu Babaiahgari
Batteries 2025, 11(10), 353; https://doi.org/10.3390/batteries11100353 - 27 Sep 2025
Abstract
With the goal of increasing energy density in lithium–ion cells, new active materials continue to be developed and evaluated. Similarly, in commercial lithium–ion cells, inert materials present in manufactured cells should also be evaluated. The impact of the thickness of inert materials on [...] Read more.
With the goal of increasing energy density in lithium–ion cells, new active materials continue to be developed and evaluated. Similarly, in commercial lithium–ion cells, inert materials present in manufactured cells should also be evaluated. The impact of the thickness of inert materials on EV-sized lithium–ion cells was evaluated. The impact of the thicknesses of the positive current collector, negative current collector, separator, and aluminum laminate package on cell properties is presented. The impact of these materials varies greatly over different cell designs, with one of the largest impacts being from a decrease in separator material thickness, especially in cells with a high number of electrode pairs, specifically, cells with a larger thickness or cells with low-capacity loadings. For high-capacity positive electrode loading, a decrease in separator thickness from 16 to 8 microns results in an increase in stack volumetric energy density from 502 to 531 Wh/L or an increase of 5.7%. Full article
(This article belongs to the Special Issue Battery Manufacturing: Current Status, Challenges, and Opportunities)
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16 pages, 2181 KB  
Article
Continuous Separation of Lithium Iron Phosphate and Graphite Microparticles via Coupled Electric and Magnetic Fields
by Wenbo Liu, Xiaolei Chen, Pengfei Qi, Xiaomin Liu and Yan Wang
Micromachines 2025, 16(10), 1094; https://doi.org/10.3390/mi16101094 - 26 Sep 2025
Abstract
Driven by the growing demand for sustainable resource utilization, the recovery of valuable constituents from spent lithium-ion batteries (LIBs) has attracted considerable attention, whereas conventional recycling processes remain energy-intensive, inefficient, and environmentally detrimental. Herein, an efficient and environmentally benign separation strategy integrating dielectrophoresis [...] Read more.
Driven by the growing demand for sustainable resource utilization, the recovery of valuable constituents from spent lithium-ion batteries (LIBs) has attracted considerable attention, whereas conventional recycling processes remain energy-intensive, inefficient, and environmentally detrimental. Herein, an efficient and environmentally benign separation strategy integrating dielectrophoresis (DEP) and magnetophoresis (MAP) is proposed for isolating the primary components of “black mass” from spent LIBs, i.e., lithium iron phosphate (LFP) and graphite microparticles. A coupled electric–magnetic–fluid dynamic model is established to predict particle motion behavior, and a custom-designed microparticle separator is developed for continuous LFP–graphite separation. Numerical simulations are performed to analyze microparticle trajectories under mutual effects of DEP and MAP and to evaluate the feasibility of binary separation. Structural optimization revealed that the optimal separator configuration comprised an electrode spacing of 2 mm and a ferromagnetic body length of 5 mm with 3 mm spacing. Additionally, a numerical study also found that an auxiliary flow velocity ratio of 3 resulted in the best particle focusing effect. Furthermore, the effects of key operational parameters, including electric and magnetic field strengths and flow velocity, on particle migration were systematically investigated. The findings revealed that these factors significantly enhanced the lateral migration disparity between LFP and graphite within the separation channel, thereby enabling complete separation of LFP particles with high purity and recovery under optimized conditions. Overall, this study provides a theoretical foundation for the development of high-performance and environmentally sustainable LIBs recovery technologies. Full article
(This article belongs to the Collection Micro/Nanoscale Electrokinetics)
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46 pages, 7184 KB  
Review
Various Technologies to Mitigate Volume Expansion of Silicon Anode Materials in Lithium-Ion Batteries
by Jihun Jang and Taegyun Kwon
Batteries 2025, 11(9), 346; https://doi.org/10.3390/batteries11090346 - 21 Sep 2025
Viewed by 619
Abstract
Silicon anodes for lithium-ion batteries (LIBs) offer exceptional theoretical capacity (~4200 mAh/g) but face critical challenges due to significant volume expansion (>300%) during lithiation, leading to mechanical degradation and rapid capacity fading. This review highlights recent advancements in mitigating these issues, including structural [...] Read more.
Silicon anodes for lithium-ion batteries (LIBs) offer exceptional theoretical capacity (~4200 mAh/g) but face critical challenges due to significant volume expansion (>300%) during lithiation, leading to mechanical degradation and rapid capacity fading. This review highlights recent advancements in mitigating these issues, including structural designs such as core–shell architectures, porous composites, and multidimensional encapsulation techniques that buffer mechanical stress and stabilize the solid electrolyte interphase (SEI). Binder innovations and hybrid material systems further enhance electrode integrity and cycling stability. While substantial progress has been made, challenges remain in scaling these solutions for commercial applications. This paper provides insights into current strategies and future directions for enabling silicon-based anodes in next-generation LIBs. Full article
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11 pages, 2071 KB  
Article
Composite Electroforming of a Binder-Free Porous Ni/S-PTh Electrode for Li–S Batteries by Combining 3D Printing, Pulse Plating, and Composite Electrodeposition
by Wassima El Mofid, Robin Arnet, Oliver Kesten and Timo Sörgel
Batteries 2025, 11(9), 343; https://doi.org/10.3390/batteries11090343 - 19 Sep 2025
Viewed by 318
Abstract
A novel process for the synthesis of binder-free, porous nickel/polythiophene-functionalized sulfur (Ni/S-PTh) composite cathodes for lithium–sulfur (Li–S) batteries is introduced in this paper. Initially, a polyvinyl butyl polymer scaffold is 3D printed, then coated with a graphite-based conducting layer, and, finally, it is [...] Read more.
A novel process for the synthesis of binder-free, porous nickel/polythiophene-functionalized sulfur (Ni/S-PTh) composite cathodes for lithium–sulfur (Li–S) batteries is introduced in this paper. Initially, a polyvinyl butyl polymer scaffold is 3D printed, then coated with a graphite-based conducting layer, and, finally, it is pulse-plated for nickel deposition to produce a high-surface-area, mechanically stable current collector. S-PTh particles are afterwards co-deposited into the Ni matrix through composite electrodeposition. After the dissolution of the polymer template, the resulting self-standing electrodes still maintain porous structure with uniform sulfur distribution and a distinct transition between the dense Ni layer and the Ni/S-PTh composite layer. Electrochemical characterization of the Ni/S-PTh composite cathodes by galvanostatic cycling at C/10 rate results in an initial specific discharge capacity of ~1120 mAh·g−1 and a specific capacity of ~910 mAh·g−1 after 200 cycles, resulting in a high capacity retention of ~81 %. For our novel approach, no steps at high temperatures or toxic solvents are involved and the need for polymer binders and conductive additives is avoided. These results demonstrate the potential of composite electrodeposition in combination with 3D printing for producing sustainable, high-performance sulfur cathodes with tunable architecture. Full article
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15 pages, 6893 KB  
Article
One-Step LCVD Fabrication of Binder-Free Porous Graphene@SiC Heterostructures for Lithium-Ion Battery Anodes
by Song Zhang, Feiyang Ji, Wei Huang, Chitengfei Zhang, Chongjie Wang, Cuicui Li, Qingfang Xu and Rong Tu
Materials 2025, 18(18), 4341; https://doi.org/10.3390/ma18184341 - 17 Sep 2025
Viewed by 305
Abstract
The potential of silicon carbide (SiC) as a promising high-capacity and stable anode material is hindered by poor electronic conductivity and slow lithium diffusion kinetics. Here, we report a one-step laser chemical vapor deposition (LCVD) process to directly synthesize porous graphene@SiC heterostructures on [...] Read more.
The potential of silicon carbide (SiC) as a promising high-capacity and stable anode material is hindered by poor electronic conductivity and slow lithium diffusion kinetics. Here, we report a one-step laser chemical vapor deposition (LCVD) process to directly synthesize porous graphene@SiC heterostructures on carbon fiber substrates. This in situ method yields an integral, binder-free electrode architecture that enhances mechanical robustness against pulverization. A critical feature of this heterostructure is the built-in electric field at the graphene–SiC interface, which is revealed by theoretical calculations to significantly accelerate charge transport and lithium-ion diffusion. The resulting anode delivers a high reversible capacity of 668 mAh·g−1 after 100 cycles at 0.1 A·g−1. More remarkably, a unique multi-stage activation mechanism is discovered, leading to an unprecedented capacity rebound to 735 mAh·g−1 after cycling at rates up to 5 A·g−1. This activation process is observed to accelerate with increasing current density in the 0.1–2 A·g−1 range. Furthermore, post-cycling analysis via XRD, TEM, and XPS confirms both the structural durability of the electrode and a reversible lithium intercalation mechanism, providing a critical foundation for the future design of high-performance LIB anodes. Full article
(This article belongs to the Section Electronic Materials)
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16 pages, 4368 KB  
Article
Quantitative Analysis Method for Full Lifecycle Aging Pathways of Lithium-Ion Battery Systems Based on Equilibrium Potential Reconstruction
by Jiaqi Yu, Yanjie Guo and Wenjie Zhang
Appl. Sci. 2025, 15(18), 10079; https://doi.org/10.3390/app151810079 - 15 Sep 2025
Viewed by 207
Abstract
High-specific-energy lithium-ion batteries face accelerated degradation and safety risks. To ensure stable and safe operation of such batteries in electric vehicles throughout their service life, this study proposes a quantitative aging mechanism analysis method based on electrode equilibrium potential reconstruction under rest conditions. [...] Read more.
High-specific-energy lithium-ion batteries face accelerated degradation and safety risks. To ensure stable and safe operation of such batteries in electric vehicles throughout their service life, this study proposes a quantitative aging mechanism analysis method based on electrode equilibrium potential reconstruction under rest conditions. First, by integrating the single-particle electrochemical model with equilibrium potential reconstruction, a quantitative mapping framework between State of Charge (SOC) and electrode lithiation concentration is established. Subsequently, to address the strong nonlinearity between equilibrium potential and lithiation concentration, the State Transition Algorithm (STA) is introduced to solve the high-dimensional coupled parameter identification problem, enhancing aging parameter estimation accuracy. Finally, the effectiveness of the proposed method was validated using a commercial NCM622/graphite power cell as the research object, and the battery’s aging pathways were analyzed using differential voltage analysis (DVA) and incremental capacity analysis (ICA) methods. Experimental results indicate that the OCV curve fitting achieved a maximum Root Mean Square Error of 0.00932, while quantitatively revealing the degradation patterns of electrode lithiation degrees during aging under both fully charged (SOC = 100%) and fully discharged (SOC = 0%) states. Full article
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18 pages, 1837 KB  
Article
Exploring Binder–Ionic Liquid Electrolyte Systems in Silicon Oxycarbide Negative Electrodes for Lithium-Ion Batteries
by Ivonne E. Monje, Nedher Sanchez-Ramírez, Laurence Savignac, Pedro H. Camargo, Steen B. Schougaard, Daniel Bélanger and Roberto M. Torresi
Electrochem 2025, 6(3), 34; https://doi.org/10.3390/electrochem6030034 - 12 Sep 2025
Viewed by 446
Abstract
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 [...] Read more.
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
(This article belongs to the Special Issue Silicon Electrochemistry: Fundamentals and Modern Applications)
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15 pages, 8341 KB  
Article
Design, Synthesis, and Characterization of a Novel Tetra-Block Copolymer for High-Performance Self-Healing Batteries
by Işık İpek Avcı Yayla, Omer Suat Taskin and Neslihan Yuca
Polymers 2025, 17(17), 2414; https://doi.org/10.3390/polym17172414 - 5 Sep 2025
Viewed by 767
Abstract
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 [...] Read more.
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
(This article belongs to the Special Issue Smart Polymers and Composites in Multifunctional Systems)
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