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

doi:10.15541/jim20240036

Abstract

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

CLC Number:

TQ912

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.

Figures/Tables 8

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]

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]

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]

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]

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]

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]

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

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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