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Progress in Chemistry 2020, Vol. 32 Issue (4): 481-496 DOI: 10.7536/PC190627 Previous Articles   Next Articles

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: Revised: Online: Published:
  • 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)
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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
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 ℃
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
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
Fig. 1 Ionic motion of Li ions in PEO polymer matrix[46] .Copyright 2005, Elsevier
Fig. 2 Design concept of rigid-flexible coupling CCPL ASPE[47]. Copyright 2014, Springer Nature
Fig. 3 Schematic illustration for PEO-LLZTO CSE[50]. Copyright 2017, Elsevier
Fig. 4 Synthesis of freestanding cross-linked HPE membrane[52].Copyright 2018, Frontiers
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
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]
Fig. 7 Schematic diagram of PEO-based composite electrolyte[58]. Copyright 2018, American Chemical Society
Fig. 8 Elastic modulus versus ionic conductivity for the [EMI][TFSI]-based PECs with various host polymer networks[64]. Copyright 2019, Elsevier
Fig. 9 The cationic polymerization mechanism initiated by B F 3 [ 66 ] . Copyright 2017, Elsevier
Fig. 10 Schematic diagram of the HMSE[67].Copyright 2019, Wiley
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
Fig. 12 (a) Synthesis of WPU dispersion, (b) process of PEO and WPU blend polymer electrolyte membranes[75].Copyright 2018, Elsevier
Fig. 13 Schematic of apparatus side-by-side electro-spinning[76]. Copyright 2019, Wiley
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
Fig. 15 Reaction of jatropha oil-based polymer electrolyte with LiClO4 in details[79]. Copyright 2016, Elsevier
Fig. 16 Synthesis of bifunctional polysiloxane[86]. Copyright 2014, Elsevier
Fig. 17 Schematic of the structure of a synthetic electrolyte[87]. Copyright 2019, Elsevier
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