机械球磨法调控硅基负极材料结构与性能的研究进展

doi:10.15541/jim20250304

无机材料学报 ›› 2026, Vol. 41 ›› Issue (5): 561-572.DOI: 10.15541/jim20250304 CSTR: 32189.14.jim20250304

机械球磨法调控硅基负极材料结构与性能的研究进展

李涵涛¹^,²(), 沈强¹^,²(), 罗国强¹^,², 王雪飞³, 高明⁴, 陈晨¹^,²^,⁴

¹ 材料复合新技术国家重点实验室武汉理工大学, 武汉 430070
² 材料科学与工程学院武汉理工大学, 武汉 430070
³ 化学化工与生命科学学院武汉理工大学, 武汉 430070
⁴ 国创高科实业集团有限公司, 武汉 430223

收稿日期:2025-07-18 修回日期:2025-09-19 出版日期:2026-05-20 网络出版日期:2025-11-11
通讯作者: 沈强, 教授. E-mail: sqqf@263.net
作者简介:李涵涛(1998-), 男, 博士研究生. E-mail: lihantao0319@163.com
基金资助:
中国工程院院地合作项目“石英产品高端化发展战略研究”(2024-DFZD-01);国创高科-武汉理工联合技术研究中心项目“先进复合材料研制”(303-612307621)

Research Progress on Structure and Performance Regulation of Silicon-based Anode Materials via Mechanical Ball Milling

LI Hantao¹^,²(), SHEN Qiang¹^,²(), LUO Guoqiang¹^,², WANG Xuefei³, GAO Ming⁴, CHEN Chen¹^,²^,⁴

¹ State Key Laboratory of Advanced Technology For Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
² School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China
³ School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China
⁴ GuoChuang Hi-Tech Industrial Group Co., Ltd., Wuhan 430223, China

Received:2025-07-18 Revised:2025-09-19 Published:2026-05-20 Online:2025-11-11
Contact: SHEN Qiang, professor. E-mail: sqqf@263.net
About author:LI Hantao (1998-), male, PhD candidate. E-mail: lihantao0319@163.com
Supported by:
Chinese Academy of Engineering Academy-Local Cooperation Project “Strategic Research on High-End Development of Quartz Products”(2024-DFZD-01);GuoChuang Hi-Tech-Wuhan University of Technology Joint Technology Research Center Project “Development of Advanced Composite Materials”(303-612307621)

摘要/Abstract

摘要：

硅因其超高的理论比容量, 被广泛认为是下一代高能量密度锂离子电池负极的理想候选材料。然而, 硅材料在实际应用中面临多种挑战, 包括在反复充放电过程中剧烈的体积膨胀、较差的电导率以及电极-电解质界面的不稳定性。机械球磨技术作为一种固态加工技术, 因其具有结构可调、操作简便和易于规模化等特点, 在改善硅基负极材料性能方面显示出巨大潜力。该技术能够精确调控颗粒尺寸、形貌和结构特性, 从而为提升材料性能提供了高效且灵活的策略, 且不需要过于复杂或苛刻的加工条件。本文综述了机械球磨技术在硅基负极材料性能调控方面的最新研究进展, 涵盖了纳米硅的可控制备、硅-碳复合材料的合理设计、硅-金属及金属硅化物复合体系的构建以及原位包覆策略的实施等方面。这些研究表明, 机械球磨技术在提升硅基负极材料的结构稳定性和电化学性能方面发挥了至关重要的作用。此外, 本文还探讨了该技术目前面临的主要挑战, 如复合材料均匀性差、球磨过程中能量输入控制复杂以及对界面反应机制的理解不足等问题。最后, 展望了该领域未来的研究方向, 包括智能球磨、界面工程和数据驱动的优化方法, 以期为高性能硅基负极材料在高能量密度锂离子电池中的应用和推广提供重要参考。

关键词: 硅, 负极材料, 机械球磨, 电化学性能, 综述

Abstract:

Silicon, due to its exceptionally high theoretical capacity, is widely regarded as an ideal candidate for the anode material in next-generation high-energy-density lithium-ion batteries. However, its practical application is limited by several critical issues, including significant volume expansion during repeated cycling, poor intrinsic conductivity, and instability at the electrode-electrolyte interface. Mechanical ball milling, a solid-state processing technique, offers significant advantages in the performance enhancement of silicon-based anode materials due to its adjustable structure, simplicity in operation, and scalability. This method enables precise control over particle size, morphology, and structural characteristics, providing an efficient and flexible strategy for improving material performance without the need for overly complex or stringent processing conditions. This review summarizes the recent progress in the application of mechanical ball milling for the performance optimization of silicon-based anode materials. Representative advancements include the controlled preparation of nanosilicon, rational design of silicon- carbon composite materials, construction of silicon-metal and metal silicide composite systems, and the implementation of in situ coating strategies. Overall, these studies clearly demonstrate that mechanical ball milling plays a key role in enhancing the structural stability and electrochemical performance of silicon-based anodes. Furthermore, this paper discusses the main challenges currently faced in this field, such as poor uniformity of composite materials, complexity of controlling energy input during milling, and limited understanding of the interface reaction mechanisms. Finally, emerging directions in the field are highlighted, including smart ball milling, interface engineering, and data-driven optimization, which are expected to provide valuable insights for the practical application and commercial promotion of high-performance silicon-based anode materials in high-energy-density lithium-ion batteries.

Key words: silicon, anode material, mechanical ball milling, electrochemical performance, review

中图分类号:

TQ174

李涵涛, 沈强, 罗国强, 王雪飞, 高明, 陈晨. 机械球磨法调控硅基负极材料结构与性能的研究进展[J]. 无机材料学报, 2026, 41(5): 561-572.

LI Hantao, SHEN Qiang, LUO Guoqiang, WANG Xuefei, GAO Ming, CHEN Chen. Research Progress on Structure and Performance Regulation of Silicon-based Anode Materials via Mechanical Ball Milling[J]. Journal of Inorganic Materials, 2026, 41(5): 561-572.

图/表 8

图1 硅电极失效机制[8]

Fig. 1 Si electrode failure mechanisms[8] (a) Material pulverization; (b) Continuous SEI growth; (c) Morphology and volume change of the entire Si electrode

表1

Table 1 Comparison of common preparation methods for silicon-based anode materials[12-21]

Method	Representative feature and advantage	Issue and limitation	Applicability/industrialization potential	Ref.
Chemical vapor deposition	Constructing high-quality core- shell structures; ensuring good film uniformity	Expensive equipment; complex process; low yield; high energy consumption	Commonly used in laboratory research; limited industrialization	[12-13]
Spray drying	Enabling batch synthesis of spherical particles; suitable for composite material fabrication	High raw material requirements; uneven particle size distribution; complex structural control	Having pilot-scale potential, but precision is limited	[14-15]
Sol-Gel method	Allowing fine control of material structure and composition; suitable for porous or composite materials	Organic precursors are complex, highly sensitive to environment; heat treatment may cause composition changes	Suitable for laboratory use; difficult to scale up	[16-17]
High-temperature carbothermal reduction	Relatively low cost; suitable for synthesizing metal silicides	High processing temperature; poor structural control; limited product purity	Having limited application scope	[18-19]
Mechanical milling	Simple equipment; low cost; enabling nanosizing; in situ compositing; easy mass production	Slightly inferior control over particle morphology; requiring prevention of agglomeration and over-grinding; some contamination must be controlled	Highest industrialization potential and broad process applicability	[20-21]

图2 不同粒径硅粉制备的硅负极的电化学性能[35]

Fig. 2 Electrochemical performance of silicon anodes prepared with silicon powders of various particle sizes[35] (a) Electrochemical performance of silicon powders with different particle sizes; (b) Scanning electron microscope (SEM) images of the fabricated anode electrode after different cycles

图3 采用湿法球磨硅片制备纳米硅粉[38]

Fig. 3 Preparation of nanosilicon powders from silicon wafers by wet ball milling[38] (a) Schematic of the wet ball milling process; (b) Electrochemical performance of the resulting nanosilicon powders

图4 硅电极的两种重要失效机制以及硅与碳材料(C@Si)复合的积极影响[45]

Fig. 4 Two important failure mechanisms of Si electrode and positive effect of compositing Si with carbon materials (C@Si)[45] (a) Pulverization of silicon particles; (b) Collapse of the entire sole silicon electrode; (c) Reduction of pulverization and increasing of cycling life in C@Si; (d) Possible healing mechanism in C@Si and a more stable contact with current collector

图5 机械球磨法制备的各类硅-碳复合材料[47,49 -50]

Fig. 5 Preparation processes of various silicon-carbon composites by mechanical ball milling[47,49 -50] (a) Schematic representation of the preparation process of Si/C composite[47]; (b) Constructing schematic diagram of the Si@Co@C[49]; (c) Schematic of the fabrication process of the present Si@APTES/f-Gr composite[50]

图6 具有嵌锂活性的元素示意图与机械球磨法制备的各种硅-金属复合材料流程图[62-64]

Fig. 6 Schematic illustration of lithiation-active elements and process flow diagrams of various silicon-metal composites prepared by mechanical milling[62-64] (a) Schematic diagram of elements with lithium intercalation activity[62]; (b) Schematic of fabrication process of the Si/TiSi2 composite[63]; (c) Preparation process of Si/FeₓSiᵧ composite powder by mechanical ball milling[64]

图7 机械球磨法在硅表面构筑无机涂层的流程图与锂化-脱锂循环后Si3N4和C涂层材料的结构演变示意图[78,80,89]

Fig. 7 Schematic illustration of the construction of inorganic coatings on silicon surfaces via mechanical milling and the structural evolution of two coating materials (Si3N4 and carbon) after lithiation-delithiation cycles[78,80,89] (a) Flowchart for preparing Si@SiOx/GNS anode materials by ball milling[78]; (b) Schematic diagram of the structural evolution of Si3N4 and carbon-coated materials after lithiation-delithiation cycles[80]; (c) Flowchart for preparing silicon nitride compounds by ball milling[89]

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机械球磨法调控硅基负极材料结构与性能的研究进展

Research Progress on Structure and Performance Regulation of Silicon-based Anode Materials via Mechanical Ball Milling

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