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Li-Ion Battery Materials
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Li-Ion Battery Materials

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Applied Chemistry".

Deadline for manuscript submissions: closed (15 March 2023) | Viewed by 19503

Special Issue Editors

Prof. Dr. Shijun Liao

E-Mail Website
Guest Editor
The Key Laboratory of Fuel Cell Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, China
Interests: sub-exchange membrane fuel cell technology; electrocatalysis; lithium-air battery; lithium-ion battery materials; other batteries: potassium ion batteries, etc.
Special Issues, Collections and Topics in MDPI journals
Dr. Xiangbo Meng

E-Mail Website
Guest Editor
Department of Mechanical Engineering, The University of Arkansas, Fayetteville, AR 72701, USA
Interests: lithium-ion batteries; lithium metal batteries; battery interface engineering
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Yuanfu Deng

E-Mail Website
Guest Editor
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China
Interests: electrochemical energy storage; Li-ion batteries; Li-metal batteries; solid-state batteries; supercapacitors
Special Issues, Collections and Topics in MDPI journals
Dr. Xiaoyuan Zeng

E-Mail Website
Guest Editor
National and Local Joint Engineering Laboratory for Lithium-Ion Batteries and Materials Preparation Technology, Key Laboratory of Advanced Battery Materials of Yunnan Province, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China
Interests: LIB materials; lithium air battery

Special Issue Information

Dear Colleagues,

Lithium-ion batteries have emerged as critical electrochemical devices, essential customable and important power sources for vehicles and large-scale energy storage systems. As one of the most important components, the materials, including positive and negative electrode materials, play a significant role for the improvement of the performance of lithium-ion batteries. Indeed, the rational design and preparation of various nanomaterials for LIB application has attracted huge attention from researchers worldwide in recent decades, and it has been a major research theme for the development of high-performance batteries. To present the achievements and progress in LIB materials in recent years, we are organizing this Special Issue.

This Special Issue on “Lithium-Ion Battery Materials” will cover the latest advancements in LIB materials, including positive electrode materials and negative electrode materials in terms of the following aspects: material design and preparation, structure characterization, exploration of new materials and preparation technologies, theoretical calculation and simulation, etc.

Prof. Dr. Shijun Liao
Dr. Xiangbo Meng
Prof. Dr. Yuanfu Deng
Dr. Xiaoyuan Zeng
Guest Editors

Manuscript Submission Information

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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. Molecules is an international peer-reviewed open access semimonthly 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

  • lithium-ion battery
  • anode materials
  • cathode materials
  • preparation
  • characterization
  • calculation and simulation

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Published Papers (7 papers)

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Research

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21 pages, 6443 KiB  
Article
Unraveling the Mechanism and Practical Implications of the Sol-Gel Synthesis of Spinel LiMn2O4 as a Cathode Material for Li-Ion Batteries: Critical Effects of Cation Distribution at the Matrix Level
by Oyunbayar Nyamaa, Gyeong-Ho Kang, Sun-Chul Huh, Jeong-Hyeon Yang, Tae-Hyun Nam and Jung-Pil Noh
Molecules 2023, 28(8), 3489; https://doi.org/10.3390/molecules28083489 - 15 Apr 2023
Cited by 7 | Viewed by 3057
Abstract
Spinel LiMn2O4 (LMO) is a state-of-the-art cathode material for Li-ion batteries. However, the operating voltage and battery life of spinel LMO needs to be improved for application in various modern technologies. Modifying the composition of the spinel LMO material alters [...] Read more.
Spinel LiMn2O4 (LMO) is a state-of-the-art cathode material for Li-ion batteries. However, the operating voltage and battery life of spinel LMO needs to be improved for application in various modern technologies. Modifying the composition of the spinel LMO material alters its electronic structure, thereby increasing its operating voltage. Additionally, modifying the microstructure of the spinel LMO by controlling the size and distribution of the particles can improve its electrochemical properties. In this study, we elucidate the sol-gel synthesis mechanisms of two common types of sol-gels (modified and unmodified metal complexes)—chelate gel and organic polymeric gel—and investigate their structural and morphological properties and electrochemical performances. This study highlights that uniform distribution of cations during sol-gel formation is important for the growth of LMO crystals. Furthermore, a homogeneous multicomponent sol-gel, necessary to ensure that no conflicting morphologies and structures would degrade the electrochemical performances, can be obtained when the sol-gel has a polymer-like structure and uniformly bound ions; this can be achieved by using additional multifunctional reagents, namely cross-linkers. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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17 pages, 3633 KiB  
Article
Ultrafine Co-Species Interspersed g-C3N4 Nanosheets and Graphene as an Efficient Polysulfide Barrier to Enable High Performance Li-S Batteries
by Shanxing Wang, Xinye Liu and Yuanfu Deng
Molecules 2023, 28(2), 588; https://doi.org/10.3390/molecules28020588 - 6 Jan 2023
Cited by 1 | Viewed by 1661
Abstract
Lithium-sulfur (Li-S) batteries are regarded as one of the promising advanced energy storage systems due to their ultrahigh capacity and energy density. However, their practical applications are still hindered by the serious shuttle effect and sluggish reaction kinetics of soluble lithium polysulfides. Herein, [...] Read more.
Lithium-sulfur (Li-S) batteries are regarded as one of the promising advanced energy storage systems due to their ultrahigh capacity and energy density. However, their practical applications are still hindered by the serious shuttle effect and sluggish reaction kinetics of soluble lithium polysulfides. Herein, g-C3N4 nanosheets and graphene decorated with an ultrafine Co-species nanodot heterostructure (Co@g-C3N4/G) as separator coatings were designed following a facile approach. Such an interlayer can not only enable effective polysulfide affinity through the physical barrier and chemical binding but also simultaneously have a catalytic effect on polysulfide conversion. Because of these superior merits, the Li-S cells assembled with Co@g-C3N4/G-PP separators matched with the S/KB composites (up to ~70 wt% sulfur in the final cathode) exhibit excellent rate capability and good cyclic stability. A high specific capacity of ~860 mAh g−1 at 2.0 C as well as a capacity-fading rate of only ~0.035% per cycle over 350 cycles at 0.5 C can be achieved. This bifunctional separator can even endow a Li-S cell at a low current density to exhibit excellent cycling capability, with a capacity retention rate of ~88.4% at 0.2 C over 250 cycles. Furthermore, a Li-S cell with a Co@g-C3N4/G-PP separator possesses a stable specific capacity of 785 mAh g−1 at 0.2 C after 150 cycles and a superior capacity retention rate of ~84.6% with a high sulfur loading of ~3.0 mg cm−2. This effective polysulfide-confined separator holds good promise for promoting the further development of high-energy-density Li-S batteries. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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15 pages, 4062 KiB  
Article
Two-Dimensional Iron Phosphorus Trisulfide as a High-Capacity Cathode for Lithium Primary Battery
by Syama Lenus, Pallavi Thakur, Sai Smruti Samantaray, Tharangattu N. Narayanan and Zhengfei Dai
Molecules 2023, 28(2), 537; https://doi.org/10.3390/molecules28020537 - 5 Jan 2023
Cited by 8 | Viewed by 2790
Abstract
Metal phosphorus trichalcogenide (MPX3) materials have aroused substantial curiosity in the evolution of electrochemical storage devices due to their environment-friendliness and advantageous X-P synergic effects. The interesting intercalation properties generated due to the presence of wide van der Waals gaps along [...] Read more.
Metal phosphorus trichalcogenide (MPX3) materials have aroused substantial curiosity in the evolution of electrochemical storage devices due to their environment-friendliness and advantageous X-P synergic effects. The interesting intercalation properties generated due to the presence of wide van der Waals gaps along with high theoretical specific capacity pose MPX3 as a potential host electrode in lithium batteries. Herein, we synthesized two-dimensional iron thio-phosphate (FePS3) nanoflakes via a salt-template synthesis method, using low-temperature time synthesis conditions in single step. The electrochemical application of FePS3 has been explored through the construction of a high-capacity lithium primary battery (LPB) coin cell with FePS3 nanoflakes as the cathode. The galvanostatic discharge studies on the assembled LPB exhibit a high specific capacity of ~1791 mAh g−1 and high energy density of ~2500 Wh Kg−1 along with a power density of ~5226 W Kg−1, some of the highest reported values, indicating FePS3′s potential in low-cost primary batteries. A mechanistic insight into the observed three-staged discharge mechanism of the FePS3-based primary cell resulting in the high capacity is provided, and the findings are supported via post-mortem analyses at the electrode scale, using both electrochemical- as well as photoelectron spectroscopy-based studies. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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14 pages, 3931 KiB  
Article
Building Polymeric Framework Layer for Stable Solid Electrolyte Interphase on Natural Graphite Anode
by Yunhao Zhao, Yueyue Wang, Rui Liang, Guobin Zhu, Weixing Xiong and Honghe Zheng
Molecules 2022, 27(22), 7827; https://doi.org/10.3390/molecules27227827 - 13 Nov 2022
Cited by 6 | Viewed by 2413
Abstract
The overall electrochemical performance of natural graphite is intimately associated with the solid electrolyte interphase (SEI) layer developed on its surface. To suppress the interfacial electrolyte decomposition reactions and the high irreversible capacity loss relating to the SEI formation on a natural graphite [...] Read more.
The overall electrochemical performance of natural graphite is intimately associated with the solid electrolyte interphase (SEI) layer developed on its surface. To suppress the interfacial electrolyte decomposition reactions and the high irreversible capacity loss relating to the SEI formation on a natural graphite (NG) surface, we propose a new design of the artificial SEI by the functional molecular cross-linking framework layer, which was synthesized by grafting acrylic acid (AA) and N,N′−methylenebisacrylamide (MBAA) via an in situ polymerization reaction. The functional polymeric framework constructs a robust covalent bonding onto the NG surface with —COOH and facilitates Li+ conduction owing to the effect of the —CONH group, contributing to forming an SEI layer of excellent stability, flexibility, and compactness. From all the benefits, the initial coulombic efficiency, rate performance, and cycling performance of the graphite anode are remarkably improved. In addition, the full cell using the LiNi0.5Co0.2Mn0.3O2 cathode against the modified NG anode exhibits much-prolonged cycle life with a capacity retention of 82.75% after 500 cycles, significantly higher than the cell using the pristine NG anode. The mechanisms relating to the artificial SEI growth on the graphite surface were analyzed. This strategy provides an efficient and feasible approach to the surface optimization for the NG anode in LIBs. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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12 pages, 2427 KiB  
Article
A Dual Functional Artificial SEI Layer Based on a Facile Surface Chemistry for Stable Lithium Metal Anode
by Yue Ma, Feng Wu, Nan Chen, Tianyu Yang, Yaohui Liang, Zhaoyang Sun, Guangqiu Luo, Jianguo Du, Yanxin Shang, Mai Feng, Ziyue Wen, Li Li and Renjie Chen
Molecules 2022, 27(16), 5199; https://doi.org/10.3390/molecules27165199 - 15 Aug 2022
Cited by 4 | Viewed by 2999
Abstract
Solid electrolyte interphase (SEI) on a Li anode is critical to the interface stability and cycle life of Li metal batteries. On the one hand, components of SEI with the passivation effect can effectively hinder the interfacial side reactions to promote long-term cycling [...] Read more.
Solid electrolyte interphase (SEI) on a Li anode is critical to the interface stability and cycle life of Li metal batteries. On the one hand, components of SEI with the passivation effect can effectively hinder the interfacial side reactions to promote long-term cycling stability. On the other hand, SEI species that exhibit the active site effect can reduce the Li nucleation barrier and guide Li deposition homogeneously. However, strategies that only focus on a separated effect make it difficult to realize an ideal overall performance of a Li anode. Herein, a dual functional artificial SEI layer simultaneously combining the passivation effect and the active site effect is proposed and constructed via a facial surface chemistry method. Simultaneously, the formed LiF component effectively passivates the anode/electrolyte interface and contributes to the long-term stable cycling performance, while the Li-Mg solid solution alloy with the active site effect promotes the transmission of Li+ and guides homogeneous Li deposition with a low energy barrier. Benefiting from these advantages, the Li||Li cell with the modified anode performs with a lower nucleation overpotential of 2.3 mV, and an ultralong cycling lifetime of over 2000 h at the current density of 1 mA cm−2, while the Li||LiFePO4 full battery maintains a capacity retention of 84.6% at rate of 1 C after 300 cycles. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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25 pages, 3930 KiB  
Article
Novel Phosphonium-Based Ionic Liquid Electrolytes for Battery Applications
by Andreas Hofmann, Daniel Rauber, Tzu-Ming Wang, Rolf Hempelmann, Christopher W. M. Kay and Thomas Hanemann
Molecules 2022, 27(15), 4729; https://doi.org/10.3390/molecules27154729 - 24 Jul 2022
Cited by 11 | Viewed by 2712
Abstract
In this study, we address the fundamental question of the physicochemical and electrochemical properties of phosphonium-based ionic liquids containing the counter-ions bis(trifluoromethanesulfonyl)imide ([TFSI]−) and bis(fluorosulfonyl)imide ([FSI]−). To clarify these structure–property as well as structure–activity relationships, trimethyl-based alkyl- and ether-containing [...] Read more.
In this study, we address the fundamental question of the physicochemical and electrochemical properties of phosphonium-based ionic liquids containing the counter-ions bis(trifluoromethanesulfonyl)imide ([TFSI]−) and bis(fluorosulfonyl)imide ([FSI]−). To clarify these structure–property as well as structure–activity relationships, trimethyl-based alkyl- and ether-containing phosphonium ILs were systematically synthesized, and their properties, namely density, flow characteristics, alkali metal compatibility, oxidative stability, aluminum corrosivity as well as their use in Li-ion cells were examined comprehensively. The variable moiety on the phosphonium cation exhibited a chain length of four and five, respectively. The properties were discussed as a function of the side chain, counter-ion and salt addition ([Li][TFSI] or [Li][FSI]). High stability coupled with good flow characteristics were found for the phosphonium IL [P1114][TFSI] and the mixture [P1114][TFSI] + [Li][TFSI], respectively. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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Review

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30 pages, 7842 KiB  
Review
Atomic and Molecular Layer Deposition as Surface Engineering Techniques for Emerging Alkali Metal Rechargeable Batteries
by Matthew Sullivan, Peng Tang and Xiangbo Meng
Molecules 2022, 27(19), 6170; https://doi.org/10.3390/molecules27196170 - 20 Sep 2022
Cited by 7 | Viewed by 2827
Abstract
Alkali metals (lithium, sodium, and potassium) are promising as anodes in emerging rechargeable batteries, ascribed to their high capacity or abundance. Two commonly experienced issues, however, have hindered them from commercialization: the dendritic growth of alkali metals during plating and the formation of [...] Read more.
Alkali metals (lithium, sodium, and potassium) are promising as anodes in emerging rechargeable batteries, ascribed to their high capacity or abundance. Two commonly experienced issues, however, have hindered them from commercialization: the dendritic growth of alkali metals during plating and the formation of solid electrolyte interphase due to contact with liquid electrolytes. Many technical strategies have been developed for addressing these two issues in the past decades. Among them, atomic and molecular layer deposition (ALD and MLD) have been drawing more and more efforts, owing to a series of their unique capabilities. ALD and MLD enable a variety of inorganic, organic, and even inorganic-organic hybrid materials, featuring accurate nanoscale controllability, low process temperature, and extremely uniform and conformal coverage. Consequently, ALD and MLD have paved a novel route for tackling the issues of alkali metal anodes. In this review, we have made a thorough survey on surface coatings via ALD and MLD, and comparatively analyzed their effects on improving the safety and stability of alkali metal anodes. We expect that this article will help boost more efforts in exploring advanced surface coatings via ALD and MLD to successfully mitigate the issues of alkali metal anodes. Full article
(This article belongs to the Special Issue Li-Ion Battery Materials)
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