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Progress in Chemistry 2019, Vol. 31 Issue (4): 613-630 DOI: 10.7536/PC180916 Previous Articles   

Special Issue: 锂离子电池

Silicon-Based and -Related Materials for Lithium-Ion Batteries

Yun Zhao1, Yuqiong Kang1, Yuhong Jin2, Li Wang1,**(), Guangyu Tian3, Xiangming He1,3,**()   

  1. 1. Institute of Nuclear & New Energy Technology, Tsinghua University, Beijing 100084, China;
    2. Beijing Guyue New Materials Research Institute, Beijing University of Technology, Beijing 100124, China
    3. State Key Laboratory of Automotive Safety and Energy, Tsinghua University, Beijing 100084, China
  • Received: Online: Published:
  • Contact: Li Wang, Xiangming He
  • About author:
    ** E-mail:(Li Wang)
    (Xiangming He)
  • Supported by:
    Ministry of Science and Technology of China(2016YFE0102200); National Natural Science Foundation of China(U1564205); Beijing Talents Project(YETP0157)
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Lithium ion batteries(LIBs) have been widely used as the energy storage system for the applications of the laptop, the communication equipment and the consumer electronics. And importantly, it will be largely used in the electrical vehicles in the near future. Silicon with a high theoretical capacity of 4200 mAh·g-1(more than 10 time of current graphite anode) is one of the most promising alternative anode material for the next generation of LIBs. However, the electrode pulverization, continuous growth of solid electrolyte interphase(SEI) and lithium consumption in silicon anode material based batteries usually happen during charge/discharge process due to its huge volume change. Moreover, the weak interaction between conventional binder and silicon anode material results in the continuous separation of silicon active material. These problems severely hinder the practical application of silicon anode material. This review systematically summarize the recent progress of silicon and its related materials for LIBs. The content includes the fabrication of silicon materials, the structure of silicon materials, binders, electrolytes and electrolyte additives. Finally, the future development direction of silicon-based materials is presented.

Key words: lithium ion battery, silicon anode, nanostructure, binder, electrolyte, additives
Table 1 The comparison of the fabrication of silicon materials with different raw materials
Method Source Price Advantages Disadvantages
SiO2(solid) Metallothermic reduction Synthesis, industry
and nature		 Low Easy to obtain, suitable for porous structures and nano particles Limited structure types,
post treatment required
TEOS(liquid) Solution method and
Metallothermic reduction		 Synthesis Low Suitable for the fabrication of different of nano structures Post treatment required
Silane and its
derivative(gas)		 Chemical vapor deposition Synthesis Expensive Growth film on different surfaces Harsh conditions required
Fig. 1 Si electrochemical lithiation and delithiation curves at room temperature and 450 ℃. Black line: theoretical voltage curve at 450 ℃. Red and green line: lithiation and delithiation of crystalline Si at room temperature, respectively[24]
Fig. 2 Scheme of fabrication of sandwich structure and its cycling performance[90]
Fig. 3 (a) Scheme of volume changes of silicon nanotube with SiO2 layer as mechanical clamping layer. The mechanical clamping layer directed the volume expasion of lithiated silicon towards inner cavity, SEI then is stable as the surface of the nanotube keeps constant during charge/discharge;(b) cycling curve of silicon nanotube and(c) rate performance[92]
Fig. 4 (a) First-cycle voltage profiles of Si/LixSi composite and Si control cells. (b) Cycling performance of graphite/coated LixSi composite and graphite control cells. (c) Schematic diagrams of the electrochemical prelithiation of SiNWs, and the internal electron and Li+ pathways during the prelithiation. (d) Schematic diagrams of chemical prelithiation of Si particles. The stable LixSi can be mixed with various anode materials and serve as an prelithiation reagent. (e) Prelithiated materials are synthesized by heating a stoichiometric mixture of M nanoparticles and Li metal under mechanical stirring[99, 100, 103, 104]
Fig. 5 Scheme of(a) cross-linked binders;(b) the interaction of binders and active materials by covalent bonding;(c) binders coated on the surface of active materials, keeping pulverized particles together without disintegration [110,111,112]
Table 2 The comparison of different binders
Interaction with current collector Interaction with the surface of Si Chemical modification Stability
PVDF Fair Poor Poor Excellent
Polysaccharide Excellent Fair Good Fair
poly(amide imide) Excellent Fair Fair Good
Polyacrylic acid Excellent Fair Excellent Poor
Self-healing binders Excellent Fair Fair Poor
Conductive binder Fair Fair Fair Good
Fig. 6 The structure of different binders
Fig. 7 (a) Possible reaction schemes with FEC as electrolyte additive;(b) schematic comparison of the mechanisms occurring at Si surface using different salts;(c) the cycling curve of SiNW electrode using different electrolyte,and the SEM images of SiNW after 30 cycles: ① EC-DMC/LiPF6; ② DMC-FEC/LiPF6; ③ EC-DMC-FEC/LiPF6;(d) Raman images of the Si electrode surface after the 10th cycle in electrolytes ①PC, ②PP1NEN-TFSA[157, 162, 165, 168]
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