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化学进展 2019, Vol. 31 Issue (4): 613-630 DOI: 10.7536/PC180916 前一篇   

所属专题： 锂离子电池

• •

锂离子电池硅基负极及其相关材料

赵云1, 亢玉琼1, 金玉红2, 王莉1,**(), 田光宇3, 何向明1,3,**()   

  1. 1. 清华大学核能与新能源技术研究院 北京 100084
    2. 北京工业大学北京古月新材料研究院 北京 100124
    3. 清华大学汽车安全与节能国家重点实验室 北京 100084
  • 收稿日期:2018-09-19 出版日期:2019-01-15 发布日期:2019-01-14
  • 通讯作者: 王莉, 何向明
  • 基金资助:
    科技部国际合作项目(2016YFE0102200); 国家自然科学基金重点项目(U1564205); 北京市英才计划项目(YETP0157)
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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:2018-09-19 Online:2019-01-15 Published:2019-01-14
  • 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)

锂离子电池是目前电脑、通讯、消费电子品以及未来电动车动力系统的主要能源。硅基负极材料因其具有较高理论比容量(4200 mAh·g-1,为石墨10倍以上),被视为最理想的下一代锂离子电池负极材料。然而硅负极在充放电过程中巨大的体积膨胀造成极片材料的粉化脱落、SEI膜的持续增长、正极锂离子的不断消耗,以及现有商业化粘结剂与硅表面较弱的相互作用等诸多缺陷,造成电池容量快速的衰减,阻碍了硅基材料在锂离子电池中的商业化应用。本文对硅基负极材料及其相关电池材料,如硅材料结构、粘结剂、电解液及添加剂等,进行了系统全面的总结。最后对硅基材料目前研究进展和未来发展方向做出总结与评述,以期为下一代硅基电池体系发展提供参考。

关键词： 锂离子电池, 硅基负极, 纳米结构, 粘结剂, 电解液, 添加剂

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
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表1 不同原料制备硅材料的对比
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
图1 硅锂在常温和高温下的电化学合金化曲线。黑线为450 ℃条件下理论电压,红线和绿线分别对应着室温条件下晶体硅嵌锂和脱锂过程[24]
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]
图2 三明治材料合成以及循环示意图[90]
Fig. 2 Scheme of fabrication of sandwich structure and its cycling performance[90]
图3 (a) 以SiO2包覆层为力学钳制层的硅纳米管再充放电过程中的体积变化。力学钳制层使得硅锂化后的体积膨胀主要朝向空心不会引起表面积的改变,从而使得材料表面的SEI在充放电过程中保持稳定;(b)循环曲线;(c)倍率曲线[92]
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]
图4 (a) 硅/预锂化硅和硅负极首圈充放电曲线对比;(b) 石墨/预锂化硅和石墨负极循环对比;(c)硅纳米线电化学预锂化示意图,和其过程中内部电子和例子传输路径;(d) 硅颗粒化学预锂化示意图, 稳定的预锂化产物LixSi可混合于各种负极材料,作为一种锂补偿试剂;(e) 通过加热搅拌化学计量活性材料与金属锂预锂化的示意图[99, 100, 103, 104]
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]
图5 (a) 黏结剂交联示意图;(b) 黏结剂与活性材料共价键作用示意图;(c) 黏结剂包覆在活性材料表面,允许材料在内部膨胀 [110,111,112]
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]
表2 不同黏结剂的对比
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
图6 不同黏结剂的结构式
Fig. 6 The structure of different binders
图7 (a) FEC作为电解液添加剂的可能反应机理;(b) 使用不同电解质对活性材料表面的影响机理示意图;(c) 不同电解液环境下纳米线循环30圈的循环曲线和第30圈时硅纳米线的SEM图:① EC-DMC/LiPF6; ② DMC-FEC/LiPF6; ③ EC-DMC-FEC/LiPF6;(d) 不同电解液条件下,硅电极循环10圈后的拉曼图: ① PC, ② PP1NEN-TFSA[157, 162, 165, 168]
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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