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Electrode Materials for Rechargeable Lithium Batteries

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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: closed (30 April 2023) | Viewed by 21038

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Prof. Dr. Wenbo Liu

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School of Mechanical Engineering, Sichuan University, Chengdu 610065, China
Interests: new functionalized micro/nanoporous metal-based materials and their applications in energy (rechargeable lithium batteries, supercapacitors, fuel cells); environmental protection (organic degradation, water treatment); catalysis (electrocatalysis, photocatalysis); sensing (biomedical sensors, electrochemical sensors); other cutting-edge applied basic research

Special Issue Information

Dear Colleagues,

With the rapid development of high-efficiency electrochemical energy storage devices, lithium-ion batteries (LIBs) have been widely applied in various industrial and civil fields, such as mobile phones, laptops, electric vehicles, smart grids, and so on. However, traditional electrode materials cannot meet the expected demands of energy and power densities in the future energy storage systems due to their extremely limited specific capacities, short lifetime and poor safety. As a result, seeking alternative high-performance electrode materials is a primary challenge for next-generation rechargeable lithium batteries (RLBs) in the future, including advanced lithium-ion batteries, lithium-metal batteries, lithium-sulfur batteries, and lithium-oxygen/air batteries.

This Special Issue on “Electrode Materials for Rechargeable Lithium Batteries” will be focused on various novel high-performance anode and cathode materials for RLBs, including aspects ranging from material design to fabrication technology, scientific understanding and potential/engineering applications.

Potential topics include, but are not limited to:

Advanced lithium-ion batteries;
Advanced lithium-metal batteries;
Advanced lithium-sulfur batteries;
Advanced lithium-oxygen/air batteries;
High-performance anode material;
High-performance cathode material;
Fabrication and synthesis;
Lithium dendrite growth and inhibition;
Polysulfides transformation;
Novel electrode structure design;
Electrode material failure;
Lithium storage mechanism;
Electrochemical performance optimization.

Prof. Dr. Wenbo Liu
Guest Editor

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Keywords

lithium-ion batteries
lithium-metal batteries
lithium-sulfur batteries
lithium-oxygen/air batteries
anode material
cathode material
lithium dendrites
polysulfides
energy/power density
cycle life and stability
safety

Published Papers (10 papers)

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Research

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14 pages, 3596 KiB

Open AccessArticle

Three-Dimensional Nanoporous CNT@Mn₃O₄ Hybrid Anode: High Pseudocapacitive Contribution and Superior Lithium Storage

by Wei Zou, Hua Fang, Tengbo Ma, Yanhui Zhao, Lixia Wang, Xiaodong Jia and Linsen Zhang

Batteries 2023, 9(7), 389; https://doi.org/10.3390/batteries9070389 - 21 Jul 2023

Cited by 1 | Viewed by 980

Abstract

A composite electrode of carbon nanotube CNT@Mn₃O₄ nanocable was successfully synthesized via direct electrophoretic deposition onto a copper foil, followed by calcination. By uniformly depositing Mn₃O₄ nanoparticles on CNTs, a nanocable structure of CNT@Mn₃O₄ can be formed, where the CNT acts as a “highway” for electrons and ions to facilitate fast transportation. Moreover, capacitive energy storage processes play a crucial role in lithium (Li) storage, especially during high scan rates. The significant contribution of capacitance is highly advantageous for the rapid transfer of Li⁺ ions, which ultimately results in an improved reversible capacity and prolonged cycle stability of the battery. A high specific capacity of 1367 mAh g⁻¹ was maintained over 300 charge–discharge cycles at a current density of 1 A g⁻¹, indicating excellent capacity retention and an extended cycle life. Furthermore, the synthesis process was facile and cost-effective, obviating the need for complex procedures such as mixing and pasting. Additionally, no binder was required, thereby enhancing battery quality efficiency. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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12 pages, 5304 KiB

Open AccessArticle

Lithiophilic Quinone Lithium Salt Formed by Tetrafluoro-1,4-Benzoquinone Guides Uniform Lithium Deposition to Stabilize the Interface of Anode and PVDF-Based Solid Electrolytes

by Yinglu Hu, Li Liu, Jingwei Zhao, Dechao Zhang, Jiadong Shen, Fangkun Li, Yan Yang, Zhengbo Liu, Weixin He, Weiming Zhao and Jun Liu

Batteries 2023, 9(6), 322; https://doi.org/10.3390/batteries9060322 - 12 Jun 2023

Viewed by 1086

Abstract

Poly(vinylidene fluoride) (PVDF)-based composite solid electrolytes (CSEs) are attracting widespread attention due to their superior electrochemical and mechanical properties. However, the PVDF has a strong polar group -CF₂-, which easily continuously reacts with lithium metal, resulting in the instability of the solid electrolyte interface (SEI), which intensifies the formation of lithium dendrites. Herein, Tetrafluoro-1,4-benzoquinone (TFBQ) was selected as an additive in trace amounts to the PVDF/Li-based electrolytes. TFBQ uniformly formed lithophilic quinone lithium salt (Li₂TFBQ) in the SEI. Li₂TFBQ has high lithium-ion affinity and low potential barrier and can be used as the dominant agent to guide uniform lithium deposition. The results showed that PVDF/Li-TFBQ 0.05 with a mass ratio of PVDF to TFBQ of 1:0.05 had the highest ionic conductivity of 2.39 × 10⁻⁴ S cm⁻¹, and the electrochemical stability window reached 5.0 V. Moreover, PVDF/Li-TFBQ CSE demonstrated superior lithium dendrite suppression, which was confirmed by long-term lithium stripping/sedimentation tests over 2000 and 650 h at a current of 0.1 and 0.2 mA cm⁻², respectively. The assembled solid-state LiNi_0.6Co_0.2Mn_0.2O₂||Li cell showed an excellent performance rate and cycle stability at 30 °C. This study greatly promotes the practical research of solid-state electrolytes. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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13 pages, 2123 KiB

Open AccessFeature PaperArticle

Carbon-Coated Si Nanoparticles Anchored on Three-Dimensional Carbon Nanotube Matrix for High-Energy Stable Lithium-Ion Batteries

by Hua Fang, Qingsong Liu, Xiaohua Feng, Ji Yan, Lixia Wang, Linghao He, Linsen Zhang and Guoqing Wang

Batteries 2023, 9(2), 118; https://doi.org/10.3390/batteries9020118 - 07 Feb 2023

Cited by 6 | Viewed by 2089

Abstract

An easy and scalable synthetic route was proposed for synthesis of a high-energy stable anode material composed of carbon-coated Si nanoparticles (NPs, 80 nm) confined in a three-dimensional (3D) network-structured conductive carbon nanotube (CNT) matrix (Si/CNT@C). The Si/CNT@C composite was fabricated via in situ polymerization of resorcinol formaldehyde (RF) resin in the co-existence of Si NPs and CNTs, followed by carbonization at 700 °C. The RF resin-derived carbon shell (~10 nm) was wrapped on the Si NPs and CNTs surface, welding the Si NPs to the sidewall of the interconnected CNTs matrix to avoid Si NP agglomeration. The unique 3D architecture provides a highway for Li⁺ ion diffusion and electron transportation to allow the fast lithiation/delithiation of the Si NPs; buffers the volume fluctuation of Si NPs; and stabilizes solid–electrolyte interphase film. As expected, the obtained Si/CNT@C hybrid exhibited excellent lithium storage performances. An initial discharge capacity of 1925 mAh g⁻¹ was achieved at 0.1 A g⁻¹ and retained as 1106 mAh g⁻¹ after 200 cycles at 0.1 A g⁻¹. The reversible capacity was retained at 827 mAh g⁻¹ when the current density was increased to 1 A g⁻¹. The Si/CNT@C possessed a high Si content of 62.8 wt%, facilitating its commercial application. Accordingly, this work provides a promising exploration of Si-based anode materials for high-energy stable lithium-ion batteries. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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12 pages, 1555 KiB

Open AccessArticle

Effect of Initial Structure on Performance of High-Entropy Oxide Anodes for Li-Ion Batteries

by Otavio J. B. J. Marques, Michael D. Walter, Elena V. Timofeeva and Carlo U. Segre

Batteries 2023, 9(2), 115; https://doi.org/10.3390/batteries9020115 - 07 Feb 2023

Cited by 5 | Viewed by 2120

Abstract

Two different high-entropy oxide materials were synthesized and studied as Li-ion battery anodes. The two materials have the same active metal constituents but different inactive elements which result in different initial crystalline structures: rock salt for (MgFeCoNiZn)O and spinel for (TiFeCoNiZn)

_{3}

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_{3}

_{4}

. Local structural studies of the metal elements in these two materials over extended electrochemical cycling reveal that the redox processes responsible for the electrode capacity are independent of the initial crystallographic structure and that the capacity is solely dependent on the initial random distribution of the metal atoms and the amount of active metals in the starting material. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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13 pages, 3992 KiB

Open AccessArticle

Molybdenum Nitride and Oxide Quantum Dot @ Nitrogen-Doped Graphene Nanocomposite Material for Rechargeable Lithium Ion Batteries

by Lixia Wang, Taibao Zhao, Ruiping Chen, Hua Fang, Yihao Yang, Yang Cao and Linsen Zhang

Batteries 2023, 9(1), 32; https://doi.org/10.3390/batteries9010032 - 31 Dec 2022

Cited by 2 | Viewed by 1854

Abstract

A multistage architecture with molybdenum nitride and oxide quantum dots (MON-QDs) uniformly grown on nitrogen-doped graphene (MON-QD/NG) is prepared by a facile and green hydrothermal route followed by a one-step calcination process for lithium ion batteries (LIBs). Characterization tests show that the MON-QDs with diameters of 1–3 nm are homogeneously anchored on or intercalated between graphene sheets. The molybdenum nitride exists in the form of crystalline Mo₂N (face-centered cubic), while molybdenum oxide exists in the form of amorphous MoO₂ in the obtained composite. Electrochemical tests show that the MON-QD/NG calcinated at 600 °C has an excellent lithium storage performance with an initial discharge capacity of about 1753.3 mAh g⁻¹ and a stable reversible capacity of 958.9 mAh g⁻¹ at current density of 0.1 A g⁻¹ as well as long-term cycling stability at high current density of 5 A g⁻¹. This is due to the multistage architecture, which can provide plenty of active sites, buffer volume changes of electrode and enhance electrical conductivity as well as the synergistic effect between Mo₂N and MoO₂. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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12 pages, 3341 KiB

Open AccessArticle

Preparing Co/N-Doped Carbon as Electrocatalyst toward Oxygen Reduction Reaction via the Ancient “Pharaoh’s Snakes” Reaction

by Jian Gao, Mengxin Zhou, Xinyao Wang, Hong Wang, Zhen Yin, Xiaoyao Tan and Yuan Li

Batteries 2022, 8(10), 150; https://doi.org/10.3390/batteries8100150 - 01 Oct 2022

Cited by 4 | Viewed by 1603

Abstract

The oxygen reduction reaction (ORR) is of great importance for clean energy storage and conversion techniques such as fuel cells and metal–air batteries (MABs). However, the ORR is kinetically sluggish, and expensive noble metal catalysts are required. The high price and limited preservation of noble metal catalysts has largely hindered the wide application of clean power sources such as fuel cells and MABs. Therefore, it is important to prepare non-expensive metal catalysts (NPMC) to cut the price of the fuel cells and MABs for wide application. Here, we report the preparation of a Co₃O₄ carried on the N-doped carbon (Co/N-C) as the ORR NPMC with a facile Pharaoh’s Snakes reaction. The gas generated during the reaction is able to fabricate the porous structure of the resultant carbon doped with heteroatoms such as Co and N. The catalyst provides a high electrocatalytic activity towards ORR via the 4-e pathway with an onset and half-wave potential of 0.98 and 0.79 V (vs. RHE), respectively, in an electrolyte of 0.1 M KOH. The onset and half-wave potentials are close to those of the commercial Pt/C. This work demonstrates the promising potential of an ancient technology for preparing NPMCs toward the ORR. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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16 pages, 3818 KiB

Open AccessArticle

Effect of x on the Electrochemical Performance of Two-Layered Cathode Materials xLi₂MnO₃–(1−x)LiNi_0.5Mn_0.5O₂

by Renny Nazario-Naveda, Segundo Rojas-Flores, Luisa Juárez-Cortijo, Moises Gallozzo-Cardenas, Félix N. Díaz, Luis Angelats-Silva and Santiago M. Benites

Batteries 2022, 8(7), 63; https://doi.org/10.3390/batteries8070063 - 29 Jun 2022

Cited by 3 | Viewed by 2607

Abstract

In our study, the cathodic material xLi₂MnO₃–(1−x)LiNi_0.5Mn_0.5O₂ was synthesized by means of the co-precipitation technique. The effect of x (proportion of components Li₂MnO₃ and LiNi_0.5Mn_0.5O₂) on the structural, morphological, and electrochemical performance of the material was evaluated. Materials were structurally characterized using X-ray diffraction (XRD), and the morphological analysis was performed using the scanning electron microscopy (SEM) technique, while charge–discharge curves and differential capacity and impedance spectroscopy (EIS) were used to study the electrochemical behavior. The results confirm the formation of the structures with two phases corresponding to the rhombohedral space group R3m and the monoclinic space group C2/m, which was associated to the components of the layered material. Very dense agglomerations of particles between 10 and 20 µm were also observed. In addition, the increase in the proportion of the LiNi_0.5Mn_0.5O₂ component affected the initial irreversible capacity and the Li₂MnO₃ layer’s activation and cycling performance, suggesting an optimal chemical ratio of the material’s component layers to ensure high energy density and long-term durability. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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Review

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27 pages, 7166 KiB

Open AccessReview

Conductive Metal–Organic Frameworks for Rechargeable Lithium Batteries

by Fengjun Deng, Yuhang Zhang and Yingjian Yu

Batteries 2023, 9(2), 109; https://doi.org/10.3390/batteries9020109 - 03 Feb 2023

Cited by 9 | Viewed by 3248

Abstract

Currently, rechargeable lithium batteries are representative of high-energy-density battery systems. Nevertheless, the development of rechargeable lithium batteries is confined by numerous problems, such as anode volume expansion, dendrite growth of lithium metal, separator interface compatibility, and instability of cathode interface, leading to capacity fade and performance degradation of batteries. Since the 21st century, metal–organic frameworks (MOFs) have attracted much attention in energy-related applications owing to their ideal specific surface areas, adjustable pore structures, and targeted design functions. The insulating characteristics of traditional MOFs restrict their application in the field of electrochemistry energy storage. Recently, some teams have broken this bottleneck through the design and synthesis of electron- and proton-conductive MOFs (c-MOFs), indicating excellent charge transport properties, while the chemical and structural advantages of MOFs are still maintained. In this review, we profile the utilization of c-MOFs in several rechargeable lithium batteries such as lithium-ion batteries, Li–S batteries, and Li–air batteries. The preparation methods, conductive mechanisms, experimental and theoretical research of c-MOFs are systematically elucidated and summarized. Finally, in the field of electrochemical energy storage and conversion, challenges and opportunities can coexist. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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25 pages, 4621 KiB

Open AccessReview

Review and Stress Analysis on the Lithiation Onset of Amorphous Silicon Films

by Kai Zhang, Erwin Hüger, Yong Li, Harald Schmidt and Fuqian Yang

Batteries 2023, 9(2), 105; https://doi.org/10.3390/batteries9020105 - 02 Feb 2023

Cited by 6 | Viewed by 2360

Abstract

This work aims to review and understand the behavior of the electrochemical lithiation onset of amorphous silicon (a-Si) films as electrochemically active material for new generation lithium-ion batteries. The article includes (i) a review on the lithiation onset of silicon films and (ii) a mechanochemical model with numerical results on the depth-resolved mechanical stress during the lithiation onset of silicon films. Recent experimental studies have revealed that the electrochemical lithiation onset of a-Si films involves the formation of a Li-poor phase (Li_0.3Si alloy) and the propagation of a reaction front in the films. The literature review performed reveals peculiarities in the lithiation onset of a-Si films, such as (i) the build-up of the highest mechanical stress (up to 1.2 GPa) during lithiation, (ii) a linear increase in the mechanical stress with lithiation which mimics the characteristics of linear elastic deformation, (iii) only a minute volume increase during Li incorporation, which is lower than expected from the number of Li ions entering the silicon electrode, (iv) the largest heat generation appearing during cycling with only a minor degree of parasitic heat contribution, and (v) an unexpected enhanced brittleness. The literature review points to the important role of mechanical stresses in the formation of the Li-poor phase and the propagation of the reaction front. Consequently, a mechanochemical model consisting of two stages for the lithiation onset of a-Si film is developed. The numerical results calculated from the mechanochemical model are in good accord with the corresponding experimental data for the variations in the volumetric change with state of charge and for the moving speed of the reaction front for the lithiation of an a-Si film of 230 nm thickness under a total C-rate of C/18. An increase in the total C-rate increases the moving speed of the reaction front, and a Li-rich phase is likely formed prior to the end of the growth of the Li-poor phase at a high total C-rate. The stress-induced phase formation of the Li-poor phase likely occurs during the lithiation onset of silicon electrodes in lithium-ion battery. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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10 pages, 1188 KiB

Open AccessReview

Research Progress of Working Electrode in Electrochemical Extraction of Lithium from Brine

by Yangyang Wang, Guangya Zhang, Guangfeng Dong and Heng Zheng

Batteries 2022, 8(11), 225; https://doi.org/10.3390/batteries8110225 - 08 Nov 2022

Cited by 3 | Viewed by 2010

Abstract

Efficient extraction of Li from brine at a low cost is becoming a key technology to solve energy and environmental problems. Electrochemical extraction of Li has become a research hotspot due to its low energy consumption, high selectivity, and environmental friendliness. LiMn₂O₄, LiFePO₄, and LiNi_1/3Co_1/3Mn_1/3O₂ are widely used as cathode materials for the electrochemical extraction of Li but they also have some drawbacks, such as a small adsorption capacity. In this paper, the principle of electrochemical Li extraction from brine is reviewed and the research progress and analysis of the above three working electrode materials is summarized. In addition, analysis of the extraction of other rare ions from the working electrode material and the effect of micro-organisms on the working electrode material is also presented. Next, the shortcomings of working electrode materials are expounded upon and the research direction of working electrode materials in electrochemical Li extraction technology are prospected. It is hoped that this paper can provide insights and guidance for the research and application of electrochemical Li extraction from brine. Full article

(This article belongs to the Special Issue Electrode Materials for Rechargeable Lithium Batteries)

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