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Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation

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A special issue of Batteries (ISSN 2313-0105). This special issue belongs to the section "Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others".

Deadline for manuscript submissions: 5 June 2025 | Viewed by 28281

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Special Issue Editors

Prof. Dr. Zhenbo Wang

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Guest Editor

1. School of Chemistry and Chemical Engineering, Harbin Institute of Technology, No. 92 West-Da Zhi Street, Harbin 150001, China
2. College of Materials Science and Engineering, Shenzhen University, Shenzhen 518060, China
Interests: chemical power sources; electrocatalysis; nano-electrode materials; battery life evaluation; density functional theory

Prof. Dr. Tingfeng Yi

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Guest Editor

1. School of Materials Science and Engineering, Northeastern University, Shenyang 110819, China
2. School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao 066004, China
3. Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province, Qinhuangdao 066004, China
Interests: lithium (sodium) ion batteries; supercapacitors; lead–acid batteries; water batteries; electrocatalysis; first-principles calculation of electrode materials

Dr. Gang Sun

E-Mail Website
Guest Editor

College of Materials Science and Engineering, Shenzhen University, Shenzhen 518071, China
Interests: Li-ion batteries; cathode materials; Li-rich materials; electrode visualization imaging analysis; Na-ion batteries

Special Issue Information

Dear Colleagues,

With the development of “low-carbon goals” and the current market growth of portable electronic products, electric vehicles, and large-scale energy storage systems, high-performance lithium-ion batteries (LIBs) have attracted extensive attention on the basis of designing and preparing new electrode materials. Additionally, a systematic and thorough understanding of the structure and chemical mechanisms of the batteries will provide other insights to develop advanced and safe electrode materials for LIBs, and guide the development of high-performance batteries This Special Issue on LIBs will focus on electrode material technologies and working mechanisms, as well as battery life evaluation.

In this Special Issue, topics of interest include, but are not limited to:

Novel lithium-ion materials: positive, negative, and electrolytes;
Electrode design;
Electrode preparation technologies;
Working and reaction mechanisms of electrode materials;
Structure and chemical evolution of electrode materials;
New in situ and online sensing principles and approaches to monitor degradation phenomena;
Battery life evaluation.

Prof. Dr. Zhenbo Wang
Prof. Dr. Tingfeng Yi
Dr. Gang Sun
Guest Editors

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Keywords

novel battery materials and technologies
Li-ion batteries
electrode design
cathode
anode
electrolyte
reaction mechanisms
in situ analysis
battery life evaluation

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Published Papers (13 papers)

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Research

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12 pages, 4129 KiB

Open AccessArticle

Structural Design of Dry-Processed Lithium-Rich Mn-Based Materials with High Loading for Enhanced Energy Density

by Yujie Ma, Haojin Guo, Tai Yang and Zhifeng Wang

Batteries 2025, 11(4), 146; https://doi.org/10.3390/batteries11040146 - 7 Apr 2025

Viewed by 426

Abstract

With the growing demand for electric vehicles and consumer electronics, lithium-ion batteries with a high energy density are urgently needed. Lithium-rich manganese-based materials (LRMs) are known for their high theoretical specific capacity, rapid electron/ion transfer, and high output voltage. Constructing electrodes with a substantial amount of active materials is a viable method for enhancing the energy density of batteries. In this study, we prepare thick LRM electrodes through a dry process method of binder fibrillation. A point-to-line-to-surface three-dimensional conductive network is designed by carbon agents with various morphologies. This structural design improves conductivity and facilitates efficient ion and electron transport due to close particle contact and tight packing. A high-loading cathode (35 mg cm⁻²) is fabricated, achieving an impressive areal capacity of up to 7.9 mAh cm⁻². Moreover, the pouch cell paired with a lithium metal anode exhibits a remarkable energy density of 949 Wh kg⁻¹. Compared with the cathodes prepared by the wet process, the dry process optimizes the pathways for e⁻/Li⁺ transport, leading to reduced resistance, superior coulombic efficiency, retention over cycling, and minimized side reaction. Therefore, the novel structural adoption of the dry process represents a promising avenue for driving innovation and pushing the boundaries for enhanced energy density for batteries. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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9 pages, 1372 KiB

Open AccessArticle

Do Silicon-Based Li-Ion Batteries Require a Time-Consuming Solid Electrolyte Interphase Formation Process?

by Sheng S. Zhang

Batteries 2025, 11(4), 122; https://doi.org/10.3390/batteries11040122 - 24 Mar 2025

Viewed by 431

Abstract

The solid electrolyte interphase (SEI) is a crucial component for ensuring the safe and long-term cycling of graphite-based Li-ion batteries. Traditionally, SEI formation requires a low current rate (0.05C–0.1C) and a moderate temperature (25–45 °C), and the same process has been widely applied in the manufacturing of silicon-based Li-ion batteries. However, silicon stores Li⁺ ions through different mechanisms than graphite, raising the question of whether such a time-consuming SEI formation process is necessary. In this work, carbon-coated SiO_x is selected as a representative silicon material, and both Li/SiO_x half-cells and SiO_x/LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) full cells are assembled and cycled at varying current rates for the first 10 cycles, followed by identical cycling conditions for the subsequent cycles. The results show that the initial current rate has a minimal impact on the long-term cycling stability of both SiO_x-based Li metal half-cells and Li-ion cells. Notably, Li-ion cells formed at higher current rates exhibit lower overall impedance than those formed at lower current rates, consequently demonstrating better rate capability. These findings suggest that the time-consuming SEI formation process may not be necessary for the manufacturing of silicon-based Li-ion batteries, potentially simplifying production and reducing processing time. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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17 pages, 4572 KiB

Open AccessArticle

Improved Self-Assembled Silicon-Based Graphite Composite Anodes for Commercially Viable High-Energy-Density Lithium-Ion Batteries

by Ruye Cong, Da-Eun Jeong, Ye-Yeong Jung, Hyun-Ho Park, Jiyun Jeon, Hochun Lee and Chang-Seop Lee

Batteries 2025, 11(3), 115; https://doi.org/10.3390/batteries11030115 - 20 Mar 2025

Viewed by 711

Abstract

Silicon-based anode materials are used to improve the performance of next-generation high-energy-density lithium-ion batteries (LIBs). However, the inherent limitations and cost of these materials are hindering their mass production. Commercial graphite can overcome the shortcomings of silicon-based materials and partially reduce their cost. In this study, a high-performance, low-cost, and environmentally friendly composite electrode material suitable for mass production was developed through optimizing the silicon content of commercial silicon–graphite composites and introducing a small amount of graphene and carbon nanofibers. This partially overcomes the inherent limitations of silicon, enhances the interface stability of silicon-based materials and the cycle stability of batteries, and reduces the irreversible capacity loss of the initial cycle. At a silicon content of 15 wt%, the initial Coulombic efficiency (ICE) of the battery was 65%. Reducing the silicon content in the composite electrode from 15% to 10% increased the ICE to 70% and improved the first lithiation and delithiation capacities. The battery exhibited excellent cycle stability at a current density of 0.1 A g⁻¹, retaining approximately 65% of its capacity after 100 cycles, good performance at various current densities (0.1–1 A g⁻¹), and an excellent reversible performance. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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13 pages, 5950 KiB

Open AccessArticle

Nickel Stabilized Si/Ni/Si/Ni Multi-Layer Thin-Film Anode for Long-Cycling-Life Lithium-Ion Battery

by Yonhua Tzeng, Yu-Yang Chiou and Aurelius Ansel Wilendra

Batteries 2025, 11(2), 46; https://doi.org/10.3390/batteries11020046 - 25 Jan 2025

Viewed by 824

Abstract

Silicon-based anodes suffer from the loss of physical integrity due to large volume changes during alloying and de-alloying processes with electrolytes. By integrating electrochemically inert, physically strong, ductile nickel layers with a multi-layered thin-film silicon anode, the long-life cycling of the Si/Ni/Si/Ni anode was demonstrated. A capacity retention of 82% after 200 cycles was measured, surpassing the performance of conventional silicon thin-film anodes. This is attributed to the effective suppression of internal local stress induced by nonuniform volume expansion by the nickel layers. These findings offer a promising pathway towards the practical implementation of high-capacity silicon-based anodes in advanced lithium-ion batteries. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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12 pages, 5238 KiB

Open AccessArticle

Simulation and Optimization of a Hybrid Photovoltaic/Li-Ion Battery System

by Xiaoxiao Yu, Juntao Fan, Zihua Wu, Haiping Hong, Huaqing Xie, Lan Dong and Yihuai Li

Batteries 2024, 10(11), 393; https://doi.org/10.3390/batteries10110393 - 6 Nov 2024

Viewed by 1414

Abstract

The coupling of solar cells and Li-ion batteries is an efficient method of energy storage, but solar power suffers from the disadvantages of randomness, intermittency and fluctuation, which cause the low conversion efficiency from solar energy into electric energy. In this paper, a circuit model for the coupling system with PV cells and a charge controller for a Li-ion battery is presented in the MATLAB/Simulink environment. A new three-stage charging strategy is proposed to explore the changing performance of the Li-ion battery, comprising constant-current charging, maximum power point tracker (MPPT) charging and constant-voltage charging stages, among which the MPPT charging stage can achieve the fastest maximum power point (MPP) capture and, therefore, improve battery charging efficiency. Furthermore, the charge controller can improve the lifetime of the battery through the constant-current and constant-voltage charging scheme. The simulation results indicate that the three-stage charging strategy can achieve an improvement in the maximum power tracking efficiency of 99.9%, and the average charge controller efficiency can reach 96.25%, which is higher than that of commercial chargers. This work efficiently matches PV cells and Li-ion batteries to enhance solar energy storages, and provides a new optimization idea for hybrid PV/Li-ion systems. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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16 pages, 4071 KiB

Open AccessArticle

Improving the Performance of LiFePO₄ Cathodes with a Sulfur-Modified Carbon Layer

by Su-hyun Kwak and Yong Joon Park

Batteries 2024, 10(10), 348; https://doi.org/10.3390/batteries10100348 - 1 Oct 2024

Cited by 1 | Viewed by 2153

Abstract

LiFePO₄ (LFP) cathodes are popular due to their safety and cyclic performance, despite limitations in lithium-ion diffusion and conductivity. These can be improved with carbon coating, but further advancements are possible despite commercial success. In this study, we modified the carbon coating layer using sulfur to enhance the electronic conductivity and stabilize the carbon surface layer via two methods: 1-step and 2-step processes. In the 1-step process, sulfur powder was mixed with cellulose followed by heat treatment to form a coating layer; in the 2-step process, an additional coating layer was applied on top of the carbon coating layer. Electrochemical measurements demonstrated that the 1-step sulfur-modified LFP significantly improved the discharge capacity (~152 mAh·g⁻¹ at 0.5 C rate) and rate capability compared to pristine LFP. Raman analyses indicated that sulfur mixed with a carbon source increases the graphitization of the carbon layer. Although the 2-step sulfur modification did not exceed the 1-step process in enhancing rate capability, it improved the storage characteristics of LFP at high temperatures. The residual sulfur elements apparently protected the surface. These findings confirm that sulfur modification of the carbon layer is effective for improving LFP cathode properties, offering a promising approach to enhance the performance and stability of LFP-based lithium-ion batteries. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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10 pages, 1009 KiB

Open AccessArticle

First Principles Study of the Phase Stability, the Li Ionic Diffusion, and the Conductivity of the Li₁₀Ge_xMo_1−xP₂S₁₂ of Superionic Conductors

by Yifang Wu, Yuanzhen Chen and Shaokun Chong

Batteries 2024, 10(10), 344; https://doi.org/10.3390/batteries10100344 - 27 Sep 2024

Cited by 1 | Viewed by 1312

Abstract

Using first-principles density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations, we performed this study on the phase stability, the intrinsic redox stability, and the Li⁺ conductivity of Li₁₀Ge_xMo_1−xP₂S₁₂ (x = 0~1) superionic conductors. Molybdenum (Mo) is expected to replace expensive germanium (Ge) to lower tmaterial costs, reduce sensitivity to ambient water and oxygen, and achieve acceptable Li⁺ conductivity. The ab initio first principle molecular dynamics simulations show that room-temperature Li⁺ conductivity is 1.12 mS·cm⁻¹ for the Li₁₀Ge_0.75Mo_0.25P₂S₁₂ compound, which is comparable to the theoretical value of 6.81 mS·cm⁻¹ and the experimental measured one of 12 mS·cm⁻¹ of the Li₁₀GeP₂S₁₂ (LGPS) structure. For Li₁₀Ge_xMo_1−xP₂S₁₂ (x = 0, 0.25, 0.5 and 1) compounds, the density of states and the projection fractional wave state density were calculated. It was found that when Ge atoms were partially replaced by Mo atoms, the band gap remained unchanged at 2.5 eV, but deep level defects appeared in Mo-substituted compounds. Fortunately, this deep level defect is difficult to ionize at room temperature, so it has no effect on the electronic conductivity of Mo substitute compounds, making Mo substitution a suitable solution for electrolyte materials. The projection fractional wave state density calculation shows that the covalent bond between Mo and S is stronger than that between Ge and S, which reduces the sensitivity of Mo-substituted compounds to water and oxygen contents in the air. In addition, the partial state density coincidence curve between Li and S elements disappears in the 25% Mo-substituted compound with energies of 4–5 eV, indicating that the Li₂S by-product is decreased. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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13 pages, 5003 KiB

Open AccessArticle

Effects of Crystalline Diamond Nanoparticles on Silicon Thin Films as an Anode for a Lithium-Ion Battery

by Yonhua Tzeng, Cheng-Ying Jhan, Shi-Hong Sung and Yu-Yang Chiou

Batteries 2024, 10(9), 321; https://doi.org/10.3390/batteries10090321 - 11 Sep 2024

Cited by 2 | Viewed by 1773

Abstract

Crystalline diamond nanoparticles which are 3.6 nm in size adhering to thin-film silicon results in a hydrophilic silicon surface for uniform wetting by electrolytes and serves as a current spreader for the prevention of a local high-lithium-ion current density. The excellent physical integrity of an anode made of diamond on silicon and the long-life and high-capacity-retention cycling performance are thus achieved for lithium-ion batteries. A specific capacity of 1860 mAh/g(si) was retained after 200 cycles of discharge/charge at an areal current density of 0.2 mA/cm². This is compared to 1626 mAh/g(si) for a thin-film-silicon anode without the additive of diamond nanoparticles. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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9 pages, 6004 KiB

Open AccessArticle

Li-Ion Batteries with a Binder-Free Cathode of Carbon Nanotubes-LiFePO₄-Al Foam

by Ying Jin, Shaoxin Wei, Zhoufei Yang, Chaojie Cui, Jin Wang, Dongliang Li and Weizhong Qian

Batteries 2024, 10(8), 261; https://doi.org/10.3390/batteries10080261 - 24 Jul 2024

Cited by 2 | Viewed by 2774

Abstract

With the increasing demand for Li resources worldwide, the easy recycling of Li-ion batteries materials becomes essential. We report a binder-free cathode consisting of carbon nanotubes (CNTs) and LiFePO₄ (LFP) nanoparticles embedded in a 3D Al network. The electrode stability depends on the CNT ratio, where 3% CNT-wrapping LFPs provide a stable structure free of detachment from Al foam, as observed on Al foil. The binder-free cathode sheet exhibited excellent performance for high-rate discharge and long-term cycle life. Materials on the cathode can be easily detached with ultrasonic treatment when immersed in organic solvent, which is advantageous for a green and high-efficiency strategy of recycling all valuable materials compared to the binder-used electrode. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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12 pages, 4537 KiB

Open AccessArticle

Multi-Layer TiO_2−x-PEDOT-Decorated Industrial Fe₂O₃ Composites as Anode Materials for Cycle-Performance-Enhanced Lithium-Ion Batteries

by Yangzhou Ma, Qi Li, Haoduo Li, Zhenfei Cai, Shuai Wang, Li Zhang, Jian Li, Guangsheng Song, Youlong Xu and Tingfeng Yi

Batteries 2023, 9(9), 481; https://doi.org/10.3390/batteries9090481 - 21 Sep 2023

Viewed by 1961

Abstract

An industrial submicron-sized Fe₂O₃ with no special shape was decorated by a multi-layer coating of oxygen-deficient TiO_2−x and conducting polymer PEDOT (poly 3,4-ethylenedioxythiophene). A facile sol–gel method followed by an EDOT polymerization process was adopted to synthesize the hierarchical coating composite. The microstructure and phase composition were characterized using an X-ray diffraction analysis (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). In particular, the existence state of PEDOT was determined using Fourier transform infrared (FT-IR) and a thermogravimetric (TG) analysis. The characterization results indicated the dual phase was well-coated on the Fe₂O₃ and its thickness was nano scale. Electrochemical characterization indicated that the multi-layer coating was helpful for significantly enhancing the cycle stability of the Fe₂O₃, and its electrochemical performance was even better than that of the single-layer coating samples. The synergistic effects of the ceramic phase and conducting polymer were demonstrated to be useful for improving electrochemical properties. The obtained FTP-24 sample exhibited a specific discharge capacity of 588.9 mAh/g after 360 cycles at a current density of 100 mA/g, which effectively improved the intrinsic cycling performance of the Fe₂O₃, with a corresponding discharge capacity of 50 mAh/g after 30 cycles. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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20 pages, 6905 KiB

Open AccessArticle

SOC Estimation Methods for Lithium-Ion Batteries without Current Monitoring

by Zhaowei Zhang, Junya Shao, Junfu Li, Yaxuan Wang and Zhenbo Wang

Batteries 2023, 9(9), 442; https://doi.org/10.3390/batteries9090442 - 29 Aug 2023

Cited by 5 | Viewed by 6356

Abstract

State of charge (SOC) estimation is an important part of a battery management system (BMS). As for small portable devices powered by lithium-ion batteries, no current sensor will be configured in BMS, which presents a challenge to traditional current-based SOC estimation algorithms. In this work, an electrochemical model is developed for lithium batteries, and three methods, including the incremental seeking method, dichotomous method, and extended Kalman filter algorithm (EKF), are separately developed to establish the framework of current and SOC estimation simultaneously. The results show that the EKF algorithm performs better than the other two methods in terms of estimation accuracy and convergence speed. In addition, the estimation error of the EKF algorithm is within ±2%, which demonstrates its feasibility. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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13 pages, 6085 KiB

Open AccessArticle

Synthesis and Performance of NaTi₂(PO₄)₃/VGCF@C Anode Composite Material for Aqueous Sodium-Ion Batteries

by Bo Ding, Mingzhu Li, Fuzhou Zheng, Yangzhou Ma, Guangsheng Song, Xiulong Guan, Yi Cao and Cuie Wen

Batteries 2023, 9(5), 265; https://doi.org/10.3390/batteries9050265 - 10 May 2023

Viewed by 3060

Abstract

This study combines self-prepared NaTi₂(PO₄)₃ (NTP) with commercial vapor-grown carbon fiber (VGCF) using a solid state calcination, then coats it with carbon to synthesize the composite anode material NaTi₂(PO₄)₃/VGCF@C (NTP/VGCF@C). The microstructure and electrochemical properties of the composite material were then analyzed using microstructure analysis and electrochemical testing equipment. Single phase NTP shows nanoparticles with a polyhedral structure, and there is good contact at the interface between the nanoparticles and the VGCFs. The carbon coating formed on the NTP particles displays a nearly 6.5 nm thick layer of amorphous carbon. From the coin-cell battery performance measurements, after 850 cycles, the composite material NTP/VGCF@C exhibits an excellent retention rate of 96.3% compared to that of the pure NTP material when the current density is 200 mA/g. As a result, the composite material and lithium manganate (denoted as LMO) were assembled into an LMO-NTP/VGCF@C aqueous sodium-ion soft pack full battery system. The full battery shows an initial capacity of 31.07 mAh at a rate of 0.5C, and a reversible discharge capacity retention rate of 95.8% after 480 cycles, exhibiting a good long-cycle stability performance. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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Review

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20 pages, 1043 KiB

Open AccessReview

Rechargeable Li-Ion Batteries, Nanocomposite Materials and Applications

by Sara El Afia, Antonio Cano, Paul Arévalo and Francisco Jurado

Batteries 2024, 10(12), 413; https://doi.org/10.3390/batteries10120413 - 26 Nov 2024

Cited by 5 | Viewed by 3233

Abstract

Lithium-ion batteries (LIBs) are pivotal in a wide range of applications, including consumer electronics, electric vehicles, and stationary energy storage systems. The broader adoption of LIBs hinges on advancements in their safety, cost-effectiveness, cycle life, energy density, and rate capability. While traditional LIBs already benefit from composite materials in components such as the cathode, anode, and separator, the integration of nanocomposite materials presents significant potential for enhancing these properties. Nanocomposites, including carbon–oxide, polymer–oxide, and silicon-based variants, are engineered to optimize key performance metrics, such as electrical conductivity, structural stability, capacity, and charging/discharging efficiency. Recent research has focused on refining these composites to overcome existing limitations in energy density and cycle life, thus paving the way for the next generation of LIB technologies. Despite these advancements, challenges related to high production costs and scalability remain substantial barriers to the widespread commercial deployment of nanocomposite-enhanced LIBs. Addressing these challenges is essential for realizing the full potential of these advanced materials, thereby driving significant improvements in the performance and practical applications of LIBs across various industries. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries: Design, Preparation, Reaction Mechanisms of Electrode Materials, and Battery Life Evaluation)

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