硅泥在锂离子电池中的应用研究进展

doi:10.15541/jim20240036

无机材料学报 ›› 2024, Vol. 39 ›› Issue (9): 992-1004.DOI: 10.15541/jim20240036

硅泥在锂离子电池中的应用研究进展

刘鹏东¹(), 王桢²^,³^,⁴, 刘永锋³, 温广武¹^,⁴()

1.山东理工大学材料科学与工程学院, 淄博 255000
2.浙江吉利控股集团有限公司博士后科研工作站, 杭州 310000
3.浙江大学材料科学与工程学院, 杭州 310000
4.山东硅纳新材料科技有限公司, 淄博 255000

收稿日期:2024-02-28 修回日期:2024-03-11 出版日期:2024-09-20 网络出版日期:2024-05-08
通讯作者: 温广武, 教授. E-mail: wengw@sdut.edu.cn
作者简介:刘鹏东(1999-), 男, 硕士研究生. E-mail: liupengdong_077@163.com
基金资助:
山东省自然科学基金(ZR2022QE244);山东省泰山产业领军项目(tscy20230621)

Research Progress on the Application of Silicon Slurry in Lithium-ion Batteries

LIU Pengdong¹(), WANG Zhen²^,³^,⁴, LIU Yongfeng³, WEN Guangwu¹^,⁴()

1. School of Materials Science and Engineering, Shandong University of Technology, Zibo 255000, China
2. Postdoctoral Research Workstation of Zhejiang Geely Holding Group Co., Ltd., Hangzhou 310000, China
3. School of Materials Science and Engineering, Zhejiang University, Hangzhou 310000, China
4. Shandong Si-Nano Materials Technology Co., Ltd., Zibo 255000, China

Received:2024-02-28 Revised:2024-03-11 Published:2024-09-20 Online:2024-05-08
Contact: WEN Guangwu, professor. E-mail: wengw@sdut.edu.cn
About author:LIU Pengdong (1999-), male, Master candidate. E-mail: liupengdong_077@163.com
Supported by:
Natural Science Foundation of Shandong Province(ZR2022QE244);Taishan Industrial Entrepreneurship Leading Talents(tscy20230621)

摘要/Abstract

摘要：

光伏切割硅废料——硅泥, 因其低成本、二维片状结构和高比容量(4200 mAh·g^-1)的优势成为300 Wh·kg^-1以上高能量密度储能电池核心硅碳负极材料的理想原料之一。然而, 硅泥存在成分复杂、粒径较大、导电性差、稳定性低和电化学性能差的问题, 需要进行系统改性处理。本文综述了硅泥在锂离子电池中的应用研究进展。首先, 分析了硅泥中金属杂质和非金属杂质对电池性能的重要影响。其中金属杂质可通过磁选和酸洗去除, 非金属杂质可通过液-液萃取和热处理去除。其次, 详细阐述了纯化后硅泥的原始性能和改性方法。通过硅泥纳米化可以抑制其膨胀, 其中包括研磨、刻蚀、电热冲击和合金-脱合金等方式; 通过直接元素掺杂硅和掺杂硅表面碳层来提高导电性; 通过构建惰性层、导电层和一定作用的官能团等表面改性提高稳定性; 还可以通过硅碳复合获得稳固的机械支撑和保护。最后, 提出了基于硅泥为原料的硅基负极面临的挑战和研发方向, 展望了未来发展前景, 旨在为硅泥变废为宝提供参考, 推动高能量密度锂离子电池快速发展。

关键词: 硅泥, 光伏切割硅废料, 废硅粉, 硅碳复合, 二维硅, 锂离子电池, 综述

Abstract:

Silicon sludge, the photovoltaic cutting silicon waste, has become one of the expected raw materials for the key silicon carbon anode materials used in high energy density batteries above 300 Wh·kg^-1 due to its low cost, two-dimensional lamellar structure and ultrahigh specific capacity (4200 mAh·g^-1). However, silicon sludge requires systematic modification because of its challenges such as complex composition, large particle size, poor electrical conductivity, low stability and poor electrochemical performance. This paper systematically reviews the application status and research progress of silicon sludge in lithium-ion batteries. Firstly, the important effects of metal and non-metal impurities on battery performance are summarized, in which metal impurities are normally removed by magnetic separation and acid pickling, and non-metallic impurities are removed by liquid-liquid extraction and heat treatment. Secondly, detailed elucidation about the initial performance and modification methods of the silicon sludge is provided. Concretely, silicon sludge can be nano-sized to reduce expansion by grinding, etching, electrothermal shock, and alloy dealloying, enhance electrical conductivity through doping the intrinsic silicon and doping the carbon layer on the silicon surface, improve stability through the construction of inert layer, conductive layer and functional group, and obtain mechanical support and protection through silicon-carbon composite. Finally, the challenges, development directions and future prospects of silicon-based anode based on silicon sludge are put forward, aiming to provide a reference for converting silicon sludge into treasure and promote the rapid development of high energy density lithium-ion batteries.

Key words: silicon sludge, photovoltaic cutting silicon waste, silicon powder waste, silicon carbon composite, two-dimensional silicon, lithium-ion battery, review

中图分类号:

TQ912

刘鹏东, 王桢, 刘永锋, 温广武. 硅泥在锂离子电池中的应用研究进展[J]. 无机材料学报, 2024, 39(9): 992-1004.

LIU Pengdong, WANG Zhen, LIU Yongfeng, WEN Guangwu. Research Progress on the Application of Silicon Slurry in Lithium-ion Batteries[J]. Journal of Inorganic Materials, 2024, 39(9): 992-1004.

图/表 8

图1 硅负极存在的问题及硅泥的来源和特征

Fig. 1 Problems of Si anode and the sources and characteristics of silicon sludge (a) Lithiation/delithiation curves of Si anode at both 450 ℃ and room temperature[5]; (b) Problems in the process of Si anode lithiation/delithiation[8]; (c) Relationship between diameter size and cracking upon lithiation of individual nano silicon[9]; (d) Schematic of the multi-wire slicing of Si ingots and the typical diamond-wire saw[10]; (e) X-ray diffraction (XRD) pattern; (f) Scanning electron microscope (SEM) image of silicon sludge[13,16]

图2 硅泥中杂质的去除方式示意图

Fig. 2 Schematic diagram of removing impurities in silicon sludge (a) Magnetic separation equipment and schematic diagram of main forces exerted on a magnetic particle[24]; (b) Flow scheme of acid pickling[27]; (c) Reaction mechanism of removal of SiO2 through heat treatment of silicon sludge with NH4F[42]

表1 纯化硅泥电极的电化学性能

Table 1 Electrochemical performance of purified silicon sludge

Current density/ (A·g^-1)	First discharge capacity/ (mAh·g^-1)	Cycle number	Capacity retention/%	Ref.
0.8	1022.9	15	9.77	[10]
0.05	3100	20	12.5	[43]
0.2	3031.6	100	1.17	[44]
0.1	1082	20	1.85	[45]
0.1	2674.5	100	0.2	[36]

图3 不同方法硅泥纳米化的原理和表征

Fig. 3 Principle and characterization of nano-sized silicon sludge by different methods (a) Schematic diagram of preparing nano silicon by ball milling[59]; (b) SEM image of nano silicon prepared by stirring ball milling[61]; (c) SEM image of nano silicon prepared by transferred arc thermal plasma[62]; (d) Schematic diagram and (e) nitrogen adsorption-desorption isotherm of nano silicon by silver-assisted chemical etching[64]; (f) Schematic diagram and (g) SEM images of nano silicon by electrothermal shock method[66]; Nano silicon prepared by calcine dealloying: (h) charge-discharge curves and (i) SEM images of cross section for the working electrodes in the fresh and during initial lithiation process[67]

图4 硅泥的掺杂改性制备示意图及电化学性能

Fig. 4 Preparative schematic diagram and electrochemical performance of doping modified silicon sludge (a) Schematic diagram of the synthesis of Si@NC-ZIF composites[70]; (b) Cycling performance and (c) electrochemical impedance spectra of Si@NC-ZIF composites and silicon sludge[70]; (d) Flow scheme of silicon graphene composites prepared by boron doping[71]

图5 硅泥表面改性原理及表征

Fig. 5 Principle and characterization of surface modification of silicon sludge (a) Cycling performance of silicon sludge with different etching concentrations of hydrofluoric acid[72]; SCNS@SiO2-2.5 composites: (b) transmission electron microscope image and (c) cross sectional SEM images of the electrodes before and after 200 cycles[72]; (d) Cycling performance of silicon carbon composites prepared by lignin and silicon sludge[73]; (e) Fourier transform infrared (FT-IR) spectra of silicon sludge surface before and after DAMO modification[76]; (f) Schematic diagram of two-step introduction of epoxy functional groups[77]; (g) Cycling performance of silicon anode with different surface groups[77]; (h) FT-IR spectra of silicon sludge surface before and after SiOx films modification[10]

图6 硅泥制备硅基复合材料概览

Fig. 6 Schematic diagram of preparation for silicon-based composites from silicon sludge

表2 不同改性方法制备的硅基负极电化学性能

Table 2 Electrochemical performance of silicon-based anode prepared by different modification methods

Modification method	Current density/(A·g^-1)	Cycle number	Discharge capacity/(mAh·g^-1)	Ref.
Nano silicon	0.1	100	1480	[59]
N-doped carbon/silicon	1	200	1139	[16]
S-doped carbon/silicon	0.5	700	686.6	[82]
Integrated electrode material	1	250	1447	[83]
Silicon/graphite/carbon composite	0.1	400	741	[45]
Porous carbon/silicon composite	0.2	200	1527	[84]
Silicon/graphene composite	0.2	300	1656	[85]
Si/C core-shell structure	0.42	200	1788.9	[86]
Si/CNTs/C core-shell structure	0.84	300	720	[87]
Si@void@C hollow structure	1	300	1164.4	[88]
Si@SiO_x/Ag composite material	0.5	200	1000	[89]
pSi/Ag/C/G composite material	1	200	972	[64]
Si/TiSi₂/G@C composite material	0.8	120	943.8	[90]

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硅泥在锂离子电池中的应用研究进展

Research Progress on the Application of Silicon Slurry in Lithium-ion Batteries

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