硅酸盐学报

液态合金/二硫化钼自修复负极材料的制备及其电化学性能

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朱传晖 ¹^,² , 郭磊 ¹^,² , 胡涛 ¹^,² , 龚兴厚 ¹^,² , 吴崇刚 ¹^,² , 郑譞 ¹^,²

硅酸盐学报 | 研究论文 2024,52(6): 2024-2031

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硅酸盐学报 |研究论文 2024 , 52 (6) : 2024 -2031

液态合金/二硫化钼自修复负极材料的制备及其电化学性能

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朱传晖¹^,², 郭磊¹^,², 胡涛¹^,², 龚兴厚¹^,², 吴崇刚¹^,², 郑譞¹^,²

作者信息

^1．湖北工业大学材料与化学工程学院，绿色轻工材料湖北省重点实验室，武汉 430068

^2．湖北隆中实验室，湖北襄阳 441002

通讯作者:

郑譞（1988—），男，博士，副教授。

作者简介:

朱传晖（2000—），男，硕士研究生。

Preparation and Eletrochemical Study of Liquid Metal/MoS₂ Self-Repairing Anode Materials for Lithium-Ion Batteries

Chuanhui ZHU¹^,², Lei GUO¹^,², Tao HU¹^,², Xinghou GONG¹^,², Chonggang WU¹^,², Xuan ZHENG¹^,²

Affiliations

^1.Hubei Provincial Key Laboratory of Green Materials for Light Industry, School of Materials and Chemical Engineering, Hubei University of Technology, Wuhan 430068, China

^2.Hubei Longzhong Laboratory, Xiangyang 441002, Hubei, China

Corresponding Author:

ZHENG Xuan (1988-), male, Ph.D., Associate Professor. E-mail: zx88@hbut.edu.cn

ZHU Chuanhui (2000-), male, Master candidate. E-mail: 102210476@hbut.edu.cn

出版时间: 2024-06-20 doi: 10.14062/j.issn.0454-5648.20230606

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摘要

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二硫化钼在可充电电池等能源存储领域具有广阔的应用前景，然而其电子导电性较差、充放电过程中易粉化和团聚等问题限制了其发展。采用水热法一步合成了液态合金（LM）和二硫化钼（MoS₂）的复合负极材料（LM@MoS₂）。通过XRD、SEM等综合表征方法对复合材料的结构和形态特性进行了研究。结果表明，液态合金通过静电吸附和配位键等方式有效结合于MoS₂，形成稳定的复合结构。此外，复合材料具有较高的可变形性和化学稳定性，促进了电极材料裂纹表面的修复，减少了内部氧化还原反应，提高了锂离子电池的循环稳定性。当LM与MoS₂质量比为2∶1时，复合材料表现出最佳性能。在0.1 A·g^-1的电流密度下，经过100次循环，复合材料的比容量稳定在656.1 mA·h·g^-1，容量保持率达74.3%，该研究为锂离子电池电极的裂纹自修复提供了新思路。

关键词

二硫化钼 / 液态合金 / 锂离子电池 / 负极材料 / 自修复

Abstract

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Introduction

Two-dimensional transition metal dichalcogenides (TMDCs) have attracted much attention due to their unique "sandwich" structure. As a typical two-dimensional layered transition metal sulfide, MoS₂ has a layered structure composed of S-Mo-S triple layers with covalent bonds. The atoms in MoS₂ layer are combined by covalent bonds, while the interaction between layers depends on the van der Waals forces. This special S—Mo—S layered structure is conductive to the rapid diffusion of lithium ions, and the intercalation of lithium ions between layers during a charging and discharging process does not affect the volume change. However, MoS₂ has some problems such as poor conductivity and easy decomposition of the structure, severely hindering the development of MoS₂ electrode materials. This paper was to composite a liquid metal (LM) with MoS₂ materials. Among them, LM has an excellent ion and electron conductivity, which can improve the conductivity of MoS₂. The moderate interlayer distance of MoS₂ can restrict LM droplets within the framework, thereby allowing LM to better exert its self-healing properties for the preparation of negative electrode materials with self-healing capabilities.

Methods

400 mg of LM was firstly added into 50 mL of N, N-Dimethylformamide (DMF), and then a certain amount of phosphomolybdic acid was added into the LM and DMF under ultrasound. Also, the required thiourea and catalyst NaBH₄ were mixed in a beaker in a molar Mo∶S ratio of 1.0∶2.6. Afterwards, the two solutions were transferred to a polytetrafluoroethylene liner and reacted at 200 ℃ for 24 h. The resulting reaction solutions were washed with deionized water, N, N-Dimethylformamide, and anhydrous ethanol, respectively. Finally, the washed materials were dried in a vacuum drying oven at 70 ℃ for 12 h to obtain the final reaction product. The prepared active material was mixed with acetylene carbon black and polyvinylidene fluoride (PVDF) in a ratio of 8∶1∶1. The material was fully ground in a ball mill in the presence of an appropriate amount of solvent N-Methyl-2-pyrrolidone (NMP) to obtain a uniformly mixed slurry. The slurry was evenly coated on a copper foil and dried in a vacuum at 70 ℃ for 12 h. The dried material was cut into 12 mm discs with a slicer as a battery negative electrode, and it was assembled into a CR2016 button battery in a glove box filled with argon. Among them, the metal lithium sheet was a counter electrode, the polypropylene porous membrane (Celgard2400) was a separator, the electrolyte solute was 1 mol·L^-1 LiPF₆, the solvent was a mixed solution of ethylene carbonate (EC), dimethyl carbonate (DMC), and ethyl methyl carbonate (EMC) in a ratio of 1∶1∶1, and the foam nickel was a gasket.

Results and discussion

The results show that the liquid metal effectively combines with MoS₂ via electrostatic adsorption and coordination bonds to form a stable composite structure. In addition, the composite material has a higher deformability and a chemical stability, promoting the repair of the crack surface of the electrode material, reducing the internal redox reaction, and improving the cycle stability of the lithium-ion battery. When a mass ratio of LM∶MoS₂ is 2∶1, the composite material shows the optimum performance. At a current density of 0.1 A·g^-1, after 100 cycles, the specific capacity of the composite material is stable at 656.1 mA·h·g^-1, the capacity retention rate reaches 74.3%, effectively improving the cycle stability of the electrode material.

Conclusions

A lithium-ion battery negative electrode material LM@MoS₂ with self-healing characteristics was prepared by a hydrothermal method. The cracks generated in the electrode during the charging and discharging process were repaired via utilizing the fluidity and high surface tension of liquid metal, effectively improving the cycle life of the electrode material. The optimum cycle stability of the electrode was obtained at a mass ratio of LM∶MoS₂ of 2∶1. The LM@MoS₂ prepared could reduce the internal redox reaction of the battery, thereby improving the electrochemical performance of the battery in the process of repeated insertion and extraction of lithium ions, reducing mechanical fractures, and improving the electrochemical performance of the battery.

Key words

molybdenum disulfide / liquid metal / lithium-ion battery / anode materials / self-repairing

引用本文

朱传晖, 郭磊, 胡涛, 龚兴厚, 吴崇刚, 郑譞. 液态合金/二硫化钼自修复负极材料的制备及其电化学性能. 硅酸盐学报, 2024 , 52 (6) : 2024 -2031 . DOI: 10.14062/j.issn.0454-5648.20230606

Chuanhui ZHU, Lei GUO, Tao HU, Xinghou GONG, Chonggang WU, Xuan ZHENG. Preparation and Eletrochemical Study of Liquid Metal/MoS₂ Self-Repairing Anode Materials for Lithium-Ion Batteries[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (6) : 2024 -2031 . DOI: 10.14062/j.issn.0454-5648.20230606

基金

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湖北省自然科学基金青年项目(2022CFB899)
国家自然科学基金青年科学基金项目(52303081)

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2024年第52卷第6期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230606

接收时间：2023-08-15
首发时间：2026-10-22
出版时间：2024-06-20

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出版历史

收稿日期：2023-08-15
修回日期：2023-10-08

基金

湖北省自然科学基金青年项目(2022CFB899)

国家自然科学基金青年科学基金项目(52303081)

作者信息

^1．湖北工业大学材料与化学工程学院，绿色轻工材料湖北省重点实验室，武汉 430068

^2．湖北隆中实验室，湖北襄阳 441002

通讯作者:

郑譞（1988—），男，博士，副教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230606

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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