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

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 15723

Special Issue Editors

Prof. Dr. Zhenbo Wang

E-Mail Website
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

E-Mail Website
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

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Batteries is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

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 (8 papers)

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Research

12 pages, 5238 KiB  
Article
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 518
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 [...] Read more.
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  
Article
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
Viewed by 821
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 [...] Read more.
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  
Article
First Principles Study of the Phase Stability, the Li Ionic Diffusion, and the Conductivity of the Li10GexMo1−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
Viewed by 719
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 Li10GexMo1−xP2S12 (x [...] Read more.
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 Li10GexMo1−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 Li10Ge0.75Mo0.25P2S12 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 Li10GexMo1−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  
Article
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
Viewed by 1045
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 [...] Read more.
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  
Article
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
Viewed by 1512
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 [...] Read more.
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  
Article
Multi-Layer TiO2−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 1702
Abstract
An industrial submicron-sized Fe2O3 with no special shape was decorated by a multi-layer coating of oxygen-deficient TiO2−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 [...] Read more.
An industrial submicron-sized Fe2O3 with no special shape was decorated by a multi-layer coating of oxygen-deficient TiO2−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  
Article
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 4 | Viewed by 5481
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 [...] Read more.
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  
Article
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 2576
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 [...] Read more.
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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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Title: Cobalt-free Lithium-Rich Cathode Materials of Lithium-ion Battery: manufacture, modification and characterization
Authors: Xiaolong Guo a, Qinjun Zhu a, Yaru Yang a, Dan Nie a, Panpan Wang a, Gang Sun a, *, Zhenbo Wang a, b*
Affiliation: a College of Materials Science and Engineering, Shenzhen University, Shenzhen 518071, China B MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Lab of Urban Water Resource and Environment, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, No.92 West-Da Zhi Street, Harbin 150001, China

Title: Predictive Insights into Structural and Electronic Properties of Lin Clusters Using CoM Polynomial with Application in 2D Porous Graphene
Author: Ali
Highlights: This study reveals effective codescriptors for predicting properties of lithium clusters and derives generalized expressions for various porous graphene structures. It establishes statistically significant predictive equations and highlights the potential of these codescriptors in designing innovative materials for advanced energy storage.

Title: Atomic-level Transformations of Lithium Iron Phosphate as a Model Ceramic Material in Vacuum-Assisted Cold Spray Environment
Authors: Collin D. Rodmyre†, Stephen Bierschenk††, Paul Mack†††, Desiderio Kovar††, and Alevtina Smirnova*†,
Affiliation: † Material Science and Engineering Program, South Dakota School of Mines, 501 E Saint Joseph St. Rapid City SD, 57701 ††Mechanical Engineering Department, University of Texas Austin, 204 E. Dean Keeton Street Austin, Texas 78712-1591 †††Thermo Fisher Scientific, East Grinstead RH19 1UB, West Sussex, UK * Chemistry, Biology, and Health Sciences Department, South Dakota School of Mines, 501 E Saint Joseph St. Rapid City SD, 57701
Abstract: Cold spray (CS) technology is known as a fast and cost-effective method for surface coating and formation of dense layers from ductile particles, such as metals, metal alloys, or metal-based composites. However, this technology experiences significant challenges in engineering of ceramic coatings because of the ductile-free nature of ceramic particles. A ceramic model compound, lithium iron phosphate, was chosen to study its ability for plastic deformation in a vacuum-assisted sub-/supersonic cold-spray environment at temperatures close to its melting point. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images demonstrate that ceramic particles after CS deposition undergoes plastic deformation and create a dense ceramic coating on a substrate surface. In-situ X-ray diffraction (XRD) analysis indicates that the model ceramic material exposed to CS in vacuum undergoes significant atomic-level transformations. The LFP particles become partially amorphous, and experience atomic-level transformations confirmed by significant shifts in binding energies for the corresponding elements (lithium, iron, phosphorous, and oxygen). Post-annealing and calendering of the deposited LFP ceramic layers increases materials crystallinity and its electrochemical performance tested in electrochemical cells with lithium metal anode.

Title: Optimizing Porosity for Lithium-Ion Diffusion in Micro-Sized Silicon Anodes
Authors: Mahesh Naikwade; Pranav Katkar; Sang-Wha Lee
Affiliation: Department of Chemical and Biological Engineering, Gachon University, 1342 Seongnam-daero, Seongnam-si 13120, Republic of Korea
Abstract: A swift lithium-ion diffusion rate in micro-sized porous silicon (m-PSi) anodes is crucial for their potential as practical anode materials in Lithium-Ion Batteries (LIBs). While research has focused on improving Li-ion diffusion through structural design, the impact of porosity on diffusion and battery performance has been underexplored. To address this, we synthesized m-PSi anodes with varying porosity using a simple Metal Assisted Chemical Etching (MACE) process and tested them electrochemically. We identified an optimal porosity of ~70.01%, achieving a high Li+ ion diffusion rate of 24 × 10⁻¹⁰ cm²/s, leading to a rate capability of 760 mAh/g at 4 A and 80% recovery. This enhanced performance is due to nanosized pores and channels facilitating capacitive-controlled Li+ ion storage, offering a guideline for designing high-energy PSi anodes for next-generation LIBs.

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