Silicon-based Anode Materials Applied in High Specific Energy Lithium-ion Batteries: a Review

doi:10.15541/jim20180347

Abstract

Abstract:

Silicon has the highest theoretical lithium insertion specific capacity, more than ten times the theoretical specific capacity of graphite electrode material, and low delithiation potential, with abundant resources and good rate characteristics, high-energy-density lithium-ion battery silicon-based materials have become hot spots in application fields such as electric vehicles and renewable energy storage systems. However, it will cause powdering and structural collapse of the silicon electrode material due to its large volume expansion effect in the process of delithiation and lithium insertion. In addition, the solid electrolyte interface (SEI) layer on the surface of silicon is repeatedly formed in the electrolyte, which increases the polarization and reduces the coulomb efficiency, eventually leading to deterioration of electrochemical performance. In order to solve the above problems and realize the commercial application of silicon electrodes. This paper systematically summarizes the work to solve the volume effect in charge and discharge process through the selection and structural design of silicon-based materials, and deeply analyzes and discusses the preparation methods, electrochemical properties and corresponding mechanisms of representative silicon-based composite materials, focusing on silicon-carbon composites and SiO_x (0<x≤2) based anode materials. Finally, the problems of silicon-based anode materials are analyzed and their prospects are prospected.

Key words: silicon-based material, anode materials, lithium-ion batteries, review

CLC Number:

TM912

Yi TAN, Kai WANG. Silicon-based Anode Materials Applied in High Specific Energy Lithium-ion Batteries: a Review[J]. Journal of Inorganic Materials, 2019, 34(4): 349-357.

Figures/Tables 14

Fig. 1 Performance comparison of common anode materials

Fig. 2 Illustration of Si volume expansion during charge and discharge[9]

Fig. 3 Schematic of the failure mechanism of silicon[13]

Fig. 4 The composite map of synthesis of CNT@mp-Si and meso-porous Si nanotube [20]

Fig. 5 Schematic of the pomegranate-inspired design[25](a) Three dimensional view and (b) simplified two-dimensional cross-section view

Fig. 6 (a) Schematic diagram of the novel core-shell Si@C@void@C, TEM images of (b) raw Si, (c) Si@SiO2@C, (d) Si@void@C, (e) Si@C, (f) Si@C@SiO2@C, and (g) Si@C@void@C[26]

Fig. 7 Scanning diagrams of (a) Ag-deposited on Si and (b, c) metal induced etching Si[28]

Fig. 8 Schematic illustration of the preparation process from Al-Si alloy to the Si/C composite[30]

Table 1 Electrochemical performance of some silicon/carbon composite anodes for lithium-ion batteries

Composite type	Si source	Carbon source	Electrochemical performance	Method	Ref.
Si/Porous-C	Nano-silicon powder	Pitch	723.8 mAh/g (1st)600 mAh/g (100 mA/g, 100 )^a	Spray drying + High-temperature pyrolysis	[35]
Si@C@RGO	Silicon powder (80 nm)	Sucrose	1599 mAh/g (1st)1517 mAh/g (100 mA/g, 100 )	Spray drying + High-temperature pyrolysis	[36]
Si/C/G	Silicon powder (325 mesh)	Phenol-formaldehyde resin (PFR)	700 mAh/g (1st)550 mAh/g (100 mA/g, 40 )	High-temperature pyrolysis	[37]
Silicon-sponge	Si wafer (>20 μm)	Acetylene	790 mAh/g (1st)726 mAh/g (100 mA/g, 300 )	Electrochemical etching+ High-temperature pyrolysis	[38]
PS@C	Si powder (5 μm)	Propylene	1980 mAh/g (1st)1287 mAh/g (100 mA/g, 100)	Chemical etching + CVD	[39]
Si/C	Al-Si alloy (2-10 μm)	Polyacrylonitrile (PAN)	952 mAh/g (1st)826.3 mAh/g (200 mA/g, 300)	Chemical etching + High-temperature pyrolysis	[30]

Fig. 9 Schematic diagram of the basic electrochemical mechanism of SiOx-based materials[46]

Fig. 10 Schematic diagram of short-circuit prelithiation treatment of metal foil circuit of batteries[50]

Fig. 11 Schematic diagram of preparation of the SiOx/Si/C[54]

Fig. 12 SEM images of (a) initial SiO@C, surface ((b) secondary electron phase, (c) back scattered) and (d) cross-section of hollow SiO@void@C material[59]

Fig. 13 Performance comparisons of common Si-based anode materials[25, 30, 35-39, 47, 53-54, 59-62]

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