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化学进展 2020, Vol. 32 Issue (4): 481-496 DOI: 10.7536/PC190627 前一篇   后一篇

• •

锂电池用全固态聚合物电解质

陈嘉苗1,3, 熊靖雯1, 籍少敏1,2, 霍延平1,2,**(), 赵经纬2,3,**(), 梁亮1,2,**()   

  1. 1. 广东工业大学轻工化工学院 广州 510006
    2. 中国科学院上海有机化学研究所 有机氟化学中国科学院重点实验室 上海 200032
    3. 广州天赐高新材料股份有限公司 广州 510700
  • 收稿日期:2019-06-25 修回日期:2019-09-21 出版日期:2020-04-05 发布日期:2020-03-30
  • 通讯作者: 霍延平, 赵经纬, 梁亮
  • 作者简介:
    ** 通信作者 Corresponding author e-mail: (Yanping Huo); (Jingwei Zhao); (Liang Liang)
  • 基金资助:
    国家自然科学基金项目(61671162, 21975055, 21975053); 广东省教育厅应用研究重大项目(2017KZDXM025)
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All Solid Polymer Electrolytes for Lithium Batteries

Jiamiao Chen1,3, Jingwen Xiong1, Shaomin Ji1,2, Yanping Huo1,2,**(), Jingwei Zhao2,3,**(), Liang Liang1,2,**()   

  1. 1. College of Light Industry and Chemical Engineering, Guangdong University of Technology, Guangzhou 510006, China
    2. Key Laboratory of Organofluorine Chemistry, CAS, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai 200032, China
    3. Guangzhou Tinci Materials Technology Co., Ltd, Guangzhou 510700, China
  • Received:2019-06-25 Revised:2019-09-21 Online:2020-04-05 Published:2020-03-30
  • Contact: Yanping Huo, Jingwei Zhao, Liang Liang
  • Supported by:
    the National Natural Science Foundation of China(61671162, 21975055, 21975053); the Key Project of Educational Commission of Guangdong Province, China(2017KZDXM025)

随着储能电源和电子产品以及电动汽车的迅速发展,开发高能量密度的锂离子电池已经成为现阶段研究的重点方向之一。目前,较广泛使用的液态锂离子电池,由于容易发生有机液态电解质的泄漏、燃烧、爆炸和短路等问题,存在非常大的安全隐患。因此,迫切需要开发能量密度更高,安全性更加好的锂离子电池。与现有的有机液态电解质相比,全固态聚合物电解质(All-solid-state polymer electrolyte,ASPE)具有理论比容量更高、结构可设计性强、易于大规模生产制造、排除了泄漏液体等体系安全性能好的优点,是一类具有广泛应用前景的电解质。ASPEs在锂离子电池中起到了主导作用,研究者们对其进行了大量的科研工作。本文结合并比较了典型的ASPEs(聚醚、聚酯、聚氨酯、聚硅氧烷)的最新科研进展以及本课题组的工作,回顾了这几种固态聚合物的发展,对高性能锂电池全固态电解质的制备设计、新型锂电池、界面调控和制备工艺成型等方面作了阐述,并对其未来的研究做出展望。

关键词： 全固态聚合物电解质, 离子电导率, 聚合物锂电池

With the rapid development of energy storage power supply, electronic products and electric vehicles, the development of high energy density lithium ion battery has become one of the key research directions. At present, more widely used liquid lithium ion battery, due to the organic liquid electrolyte leakage, combustion, explosion, short circuit and other problems, poses a very big potential safety hazard. Therefore, there is an urgent need to develop lithium ion batteries with higher energy density and better safety. Compared with the existing organic liquid electrolyte, the all-solid-state polymer electrolyte (ASPE) have the advantages of higher theoretical specific capacity, stronger structural design, easier large-scale production and manufacture, and better system safety performance, which is a kind of electrolyte with wide application prospects. ASPE has played a leading role in lithium ion batteries, and researchers have done a lot of research work. This paper combines the latest scientific research progress of typical ASPE (polyether, polyester, polyurethane, polysiloxane) and the work of our group, and reviews the development of these solid polymers to develop high-performance lithium batteries. The preparation of solid electrolyte, new lithium battery, interface regulation, preparation process and other aspects have been expounded, and its future research is prospected.

Contents

1 Introduction

2 All solid polymer electrolyte theory

3 All solid polymer electrolyte

3.1 Polyether

3.2 Polyester

3.3 Polyurethane

3.4 Polysiloxane

4 Conclusion and outlook

Key words: all-solid polymer electrolytes(ASPE), ionic conductivity, polymer lithium battery
()
表1 全固态电解质的优势
Table 1 Solid state battery advantage
Index Performance
High theoretical energy density Key indicators can reach 300~400 Wh/kg
High security performance Replacing electrolytes and separators in traditional lithium-ion batteries with solid electrolytes
Wide operating temperature range -25 ℃~-60 ℃
表2 目前商业化的全固态电解质的研究情况
Table 2 Research status of commercialized all-solid electrolytes
All solid state battery research and development organization Type of battery Key indicator Battery capacity Application status
Batscap-Bolloré Li/PEO/LFP 220 Wh/kg,1500 cycle,96% 10~30 Ah Successfully applied to the French EV shared service car “Autolib” and the small bus “Bluebus”, the car currently has more than 4,000 vehicles.
Sakti3 Li/LiPON/LCO 1000 Wh/L 10~50 mAh Special field application.
Toyota Li/LPS/LCO
Li/LPS/NCM		 230 Wh/kg 2.4~15 Ah Small flatbed trial phase.
No large-scale promotion. Expected listed in 2022.
Qingdao Institute of Energy, Chinese Academy of Sciences Li/LLZO@PEO/NCM 297 Wh/kg 10 Ah Development phase
Ningbo Institute of Materials, Chinese Academy of Sciences GP/Oxide solid
electrolyte/NCM		 240 Wh/kg, 500 cycle,
88.7%
4 Ah		 Pilot line construction is underway
Qing Tao GP/Oxide solid
electrolyte/NCM		 220 Wh/kg,
1000 cycle		 5.6 Ah Pilot line construction is underway
Weilan New Energy Silicon carbon anode @Li/in situ solid state
Electrolyte/NCM		 >300 Wh/kg 1.8~42 Ah Pilot line construction is underway
Solid Power Li/LPS/S 300 Wh/L 1~5 Ah Development phase
表3 全固态电解质的汇总
Table 3 Summary of all solid electrolytes
Classification SPE Ionic conductivity
(S/cm)		 Electrochemical window(V) Thermal decomposition
temperature(℃)		 ref
Polyether PEGBCDMA/EC/LiTFSI 8.0×10-4, RT 4.5 220 8
CCPL 3.0×10-4, 60 ℃
1.4×10-3, 160 ℃		 4.6 — 47
PEO/PEI/LiClO4 1.0×10-4, RT — — 48
LiFSI/PEO 1.3×10-3, 80 ℃ 5.3 — 49
PEO/LLZTO/PEG > 10-4, 55 ℃
1.58×10-3, 80 ℃		 5.0 — 50
PVDF-HFP-Li6.5La3Zr1.5Ta0.5O12
PVDF-HFP-Li6.4La3Zr1.4Nb0.6O12 		8.8×10-5, RT
6.8×10-5, RT		 — — 51
5 wt% POSS/HPE 1.39×10-3, 80 ℃ 5.0 298 52
PMHSnC-B 1.0×10-3 , RT 4.5 500 53
LATP/PAN/PEO-LiTFSI 6.5×10-4, 60 ℃ 5.0 — 58
5 wt%LLZO/PAN-LiClO4 1.31×10-4, RT — — 59
Polyester 10 wt% PVDF/90 wt% [EMI][TFSI] 4.9×10-3, 60 ℃ — — 64
C-PEGDE 8.9×10-5, RT 4.5 — 66
PAN/LAGP/PEGDA 3.7×10-4, RT 5.0 — 67
PFCA-CPE 1.24×10-3, RT 5.0 — 68
PPC/Li6.75La3Zr1.75Ta0.25O12 5.2×10-4, 20 ℃ 4.6 — 70
PCL 4.1×10-5, 25 ℃
1.1×10-4, 40 ℃		 — — 71
CPPC 3.0×10-4, 20 ℃
1.4×10-3, 120 ℃		 4.6 — 72
Polyurethane PEO/WPU/LiTFSI 8.2×10-4, 60 ℃
3.1×10-3, 80 ℃		 4.8 336 76
TPU/PI 5.06×10-3, RT — — 77
SiO2 /PEI-PU 2.33×10-3, RT — — 79
PU/MDI/LiClO4 1.29×10-4, 30 ℃ 4.8 80
Single ion conducting P(STFSILi)-PEO-P (STFSILi) 1.3×10-5, 60 ℃ 5.0 — 54
LiPSsTFSI/PEO 1.0×10-4, 70 ℃ — — 16
Polysiloxane VC-PMHS 1.55×10-4, 25 ℃ — — 87
1.5×10-3, 100 ℃
Polysiloxane/Polyether-based 1.5×10-4, RT — — 90
图1 锂离子在PEO聚合物基体中的离子运动[46]
Fig. 1 Ionic motion of Li ions in PEO polymer matrix[46] .Copyright 2005, Elsevier
图2 刚柔耦合CCPL固体聚合物电解质的设计[47]
Fig. 2 Design concept of rigid-flexible coupling CCPL ASPE[47]. Copyright 2014, Springer Nature
图3 PEO/LLZTO/LiTFSI在不同比例的ASPEs示意图[50]
Fig. 3 Schematic illustration for PEO-LLZTO CSE[50]. Copyright 2017, Elsevier
图4 独立交联HPE膜的合成[52]
Fig. 4 Synthesis of freestanding cross-linked HPE membrane[52].Copyright 2018, Frontiers
图5 (a)聚硅氧烷网状SPE薄膜照片;(b)组装LiNi0.8Co0.2O2/SPEs/Li电池在3.0~4.1 V的循环性能[53]
Fig. 5 (a) Photograph of polysiloxane network SPE film; (b) Specific discharge capacity of the LiNi0.8Co0.2O2/SPEs/Li cell with the voltage range of 3.0~4.1 V according to cycles[53]. Copyright 2003, Elsevier
图6 作为锂金属电池电解质的单离子导体三嵌段共聚物P(STFSILi)-b-PEO-b-P(STFSILi)的化学结构[54]
Fig. 6 Chemical structure of the single-ion conductor triblock copolymer P(STFSILi)-b-PEO-b-P(STFSILi) proposed as an electrolyte for lithium-metal-based batteries[54]
图7 PEO基复合电解质的示意图[58]
Fig. 7 Schematic diagram of PEO-based composite electrolyte[58]. Copyright 2018, American Chemical Society
图8 具有各种主体聚合物网络的基于[EMI][TFSI]的PEC的弹性模量与离子电导率的关系[64]
Fig. 8 Elastic modulus versus ionic conductivity for the [EMI][TFSI]-based PECs with various host polymer networks[64]. Copyright 2019, Elsevier
图9 由BF3引发的阳离子聚合机理[66]
Fig. 9 The cationic polymerization mechanism initiated by B F 3 [ 66 ] . Copyright 2017, Elsevier
图10 HMSE的原理图[67]
Fig. 10 Schematic diagram of the HMSE[67].Copyright 2019, Wiley
图11 (a)软包电池运行良好时和(b)软包电池被切除一个小角后给LED灯供电;(c)缺角软电池的电压检测;(d)切下来的小角给LED灯供电[71]
Fig. 11 Illustration of solid-state soft-package lithium cells(a) On the well-running and (b) Being cut away for powering a red LED lamp; (c) Voltage monitoring of obtained incomplete battery; (d) The obtained corner of the cell for lighting a LED lamp[71]. Copyright 2015, Wiley
图12 (a)WPU分散体的合成,(b)PEO和WPU共混物聚合物电解质膜的方法的示意图[75]
Fig. 12 (a) Synthesis of WPU dispersion, (b) process of PEO and WPU blend polymer electrolyte membranes[75].Copyright 2018, Elsevier
图13 并排电纺丝装置原理图[76]
Fig. 13 Schematic of apparatus side-by-side electro-spinning[76]. Copyright 2019, Wiley
图14 (a)Celgard,PEI-PU和SiO2/PEI PU复合膜的Li/LiFePO4电池以0.2 C速率的循环稳定性;(b)Celgard,PEI-PU和SiO2/PEI PU复合膜以0.2 C速率的库仑效率[78]
Fig. 14 (a) Cycling stabilities of Li/LiFePO4 cells using Celgard, PEI-PU and SiO2/PEI PU composite membranes at 0.2 C rate. (b) Coulombic efficiency as a function of cycle number at 0.2 C rate[78]. Copyright 2015, Elsevier
图15 麻风树油基聚合物电解质与LiClO4反应过程[79]
Fig. 15 Reaction of jatropha oil-based polymer electrolyte with LiClO4 in details[79]. Copyright 2016, Elsevier
图16 双官能团聚硅氧烷的合成[86]
Fig. 16 Synthesis of bifunctional polysiloxane[86]. Copyright 2014, Elsevier
图17 合成电解质的结构示意图[87]
Fig. 17 Schematic of the structure of a synthetic electrolyte[87]. Copyright 2019, Elsevier
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锂电池用全固态聚合物电解质