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化学进展 2020, Vol. 32 Issue (7): 1003-1014 DOI: 10.7536/PC191005 前一篇   

• 综述 •

高安全、高比能固态锂硫电池电解质

李栋1, 郑育英1, 南皓雄1, 方岩雄1, 刘全兵1,**(), 张强2,**()   

  1. 1. 广东工业大学轻工化工学院 广州 510006
    2. 清华大学化学工程系 北京 100084
  • 收稿日期:2019-10-11 出版日期:2020-07-24 发布日期:2020-07-10
  • 通讯作者: 刘全兵, 张强
  • 基金资助:
    国家自然科学基金基金项目(U1801257); 国家自然科学基金基金项目(21606050); 国家自然科学基金基金项目(21975056); 珠江科技新星项目(201806010039); 广东省普通高校特色创新项目(2017KTSCX055)
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Electrolyte for Solid Lithium-Sulfur Batteries with High Safety and High Specific Energy

Dong Li1, Yuying Zheng1, Haoxiong Nan1, Yanxiong Fang1, Quanbing Liu1,**(), Qiang Zhang2,**()   

  1. 1. School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China
    2. Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
  • Received:2019-10-11 Online:2020-07-24 Published:2020-07-10
  • Contact: Quanbing Liu, Qiang Zhang
  • About author:
    ** e-mail:(Quanbing Liu);
    (Qiang Zhang)
  • Supported by:
    National Natural Science Foundation of China(U1801257); National Natural Science Foundation of China(21606050); National Natural Science Foundation of China(21975056); Zhujiang Science and Technology New Star Project(201806010039); Characteristic Innovation Projects of Colleges in Guangdong Province(2017KTSCX055)

锂硫电池具有理论能量密度高、成本低廉和环境友好等优点,是最有前途的下一代高比能二次电池系统之一。当前,基于有机电解液的液态锂硫电池存在多硫化锂穿梭效应、电解液易燃以及锂枝晶等问题,致使电池的库仑效率低、循环性能差,且存在严重的安全隐患。采用固态电解质(如凝胶聚合物、固态聚合物、陶瓷、复合电解质等)替代有机电解液是解决上述问题的有效途径。本文总结了近年来固态锂硫电池电解质的研究现状,评述了各类固态电解质的优缺点及改性策略,重点介绍了陶瓷固态电解质的研究进展。最后,对固态锂硫电池的未来发展趋势进行预测与展望。

关键词： 固态锂硫电池, 固态电解质, 改性, 陶瓷固态电解质

Lithium-sulfur batteries have the advantages of high theoretical energy density, low cost and environmental friendliness, and they are the most promising next-generation high-energy density secondary battery systems. Currently, liquid lithium-sulfur batteries based on organic electrolytes have some problems such as lithium polysulfides(LiPSs) shuttle effect, electrolyte flammability and lithium dendrite, resulting in low coulombic efficiency and poor cycle stability of lithium-sulfur batteries, and there are serious safety hazards. The uses of solid electrolytes(gel polymers, solid polymers, ceramics, composite electrolytes, etc.) in place of organic liquid electrolytes are effective strategies to address the above problems. Herein, we present the research status of solid-state electrolytes of lithium-sulfur batteries, and summarize their advantages/disadvantages and improvement strategies, and focuses on the research progress of ceramic solid electrolytes. Finally, we forecast future development trends of solid lithium-sulfur batteries.

Contents

1 Introduction

2 Solid electrolytes

2.1 Gel polymer electrolytes

2.2 Solid-state polymer electrolytes

2.3 Ceramic electrolytes

2.4 Composite electrolytes

3 Conclusion and outlook

Key words: solid-state lithium-sulfur batteries, solid electrolytes, modified, ceramics solid electrolytes
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图1 锂离子在PPZr-GPE膜上的迁移和抑制多硫化物机理说明[18]
Fig.1 Schematic illustration of Li+ ion transport and polysulfide blocking mechanism for the membrane of PPZr-GPE[18]. Copyright 2017, Royal Society of Chemistry.
图2 基于多功能PDA-PVDF固态锂硫电池示意图[19]
Fig.2 Scheme of the multifunction of PDA-PVDF for quasi-solid-state Li-S battery[19]. Copyright 2018, Royal Society of Chemistry.
图3 (a)LiFSI有助于形成稳定的界面层[28],(b)Al2O3包覆LATP固态聚合物电解质的制备和全固态锂硫电池结构图[30],(c)HNT添加剂提高离子电导率机理图[35]
Fig.3 (a) LiFSI helps the forming of stable interface layer[28]. Copyright 2017, American Chemical Society.(b) Schematic diagram showing the preparation of an ALD coated LATP SSE and the configuration of ASSLSBs[30]. Copyright 2018, Royal Society of Chemistry.(c) Schematic mechanism of HNT addition for enhanced ionic conductivity[35]. Copyright 2017, Elsevier.
图4 陶瓷电解质晶体结构示意图,(a) Li6PS5Cl[46],(b) Li9.54Si1.74P1.44S11.7C l 0.3 [ 64 ] ,(c) Li10GeP2 S 12 [ 65 ] ,(d) NaSICON[63],(e) Li3 x La2/3- x Ti O 3 [ 66 ] ,(f) Li7La3Zr2 O 12 [ 67 ]
Fig.4 Crystal structure of (a) Li6PS5Cl[46]. Copyright 2019, Royal Society of Chemistry. (b) Li9.54Si1.74P1.44S11.7C l 0.3 [ 64 ] . Copyright 2018, Wiley. (c) Li10GeP2 S 12 [ 65 ] . Copyright 2016, American Chemical Society. (d) NaSICON[63]. Copyright 2014, American Chemical Society. (e) Li3 x La2/3- x Ti O 3 [ 66 ] . Copyright 2003, American Chemical Society. (f) Li7La3Zr2 O 12 [ 67 ] . Copyright 2013, American Chemical Society.
图5 (a)夹层结构电解质的电池示意图;(b)锂硫电池基于不同电解质的充放电曲线图[76](c)混合电解质锂硫电池结构示意图;(d)不同浓度LLZO纳米复合材料对离子电导率的影响[1]
Fig.5 (a) Sketch of the cell with a bilayer electrolyte configuration;(b) Discharge/charge profiles of the Li-S battery with different electrolytes[76].(c) Schematic illustration of an all solid-state Li-S battery based on hybrid electrolytes;(d) Arrhenium plots of the conductivity of nanocomposite LLZO-PEO-LiClO4 with different LLZO concentrations[1]. Copyright 2017, American Chemical Society.
图6 (a) LPS-PEO-LiClO4复合固态电解质的工艺流程图;(b)LPS-PEO-LiClO4固态锂硫电池结构示意图[77]
Fig.6 (a) Schematic of fabrication process of LPS-PEO-LiClO4 hybrid solid electrolyte,(b) Schematic illustration of an all solid-state Li-S battery structure based on LPS-PEO-LiClO4 hybrid solid electrolyte[77]. Copyright 2018, American Chemical Society.
表1 不同固态电解质对锂硫电池电化学性能的影响
Table 1 The electrochemical performances of Li-S batteries with various solid-state electrolytes
Classification Molecular formula Ionic conductivity
(S·cm-1)		 Electrochemical property ref
Current density Initial capacity
(mAh·g-1)		 Cycle performance
(mAh·g-1)
Gel PDA-PVDF — 0.1 C 1215.4 200th, 868.8 19
PVDF/PEO/ZrO2 5.25×10-4(25 ℃) 0.2 C 1429 200th, 936.1 18
PVDF-HFP 6.61×10-4(20 ℃) 0.5 C 601 100th, 503 82
PETEA 1.13×10-2(25 ℃) 0.1 C 1219.8 100th, 744.1 83
PVDF/PMMA/PVDF 1.95×10-3(25 ℃) 200 mA·g-1 1711.8 50th, 1145.3 84
PEO 1.76×10-3(25 ℃) 0.1 C 1182 100th, 648 85
Solid-state polymer PEO/Al2O3-LATP/PEO 4.8×10-4(60 ℃) 0.1 C 1035 100th, 823 30
PEO/Li10SnP2S12 1.69×10-4(50 ℃) 0.2 C 330 50th, 800 34
PEO/LiFSI 9.0×10-5(70 ℃) 0.05C 900 50th, 750 28
PEO/LiTFSI/MMT 3.22×10-4(60 ℃) 0.1 C 998 100th, 634 29
PEO-LiTFSI-HNT 1.1×10-4(25 ℃) 4 C 809 400th, 386 35
Ceramic Li6PS5Cl 3.15×10-3(25 ℃) 0.176 mA·cm-2 1850 50th, 1393 45
Li9.54Si1.74P1.44S11.7Cl0.3 1.6×10-2(25 ℃) 80 mA·g-1 969 60th, 827 61
Li7P2.9S10.85Mo0.01 4.8×10-3(25 ℃) 0.05 C 1020 30th, 400 86
LLZTO-MgO 5×10-4(25 ℃) 0.2 C 1130 200th, 685 87
Li7P2.9Mn0.1S10.7I0.3 5.6×10-3(25 ℃) 0.05 C 791.6 60th, 800 11
Composite LPS-PEO-LiClO4 2.1×10-3(25 ℃) 0.05 C 826 60th, 394 77
LLZO-PEO-LiClO4 1.9×10-3(70 ℃) 0.05 mA·cm-2 >900 90th, 810 1
LICGC-CPE 6×10-4(90 ℃) 0.05 C 1111 50th, 518 76
FDE-LAGP 3.2×10-4(25 ℃) 1 C 915 1200th, 668 13
表2 用于锂硫电池的不同类型固态电解质参数及优缺点比较列表
Table 2 Comparison of advantages and disadvantages of various SSEs electrolytes for lithium-sulfur batteries
Classification Materials Transference
number(n)		 Conductivity
(S·cm-1)		 Voltage
stability		 Activation
energy
(KJ·mol-1)		 Advantage Disadvantage ref
Gel PVdF-2%SiO2 0.31 10-4~10-2 3~5.1 V 2.193 High ionic conductivity Severe Li dendrite growth 88
PVDF/PEO/ZrO2 0.71 / 1.7~6 V / Low interfacial impedance Severe LiPSs shuttling 18
PEO-TEGDME/DIOX 0.78 / 1~4 V / / Poor mechanical strength 23
Solid-state Polymer PEO/Li10SnP2S12 0.38 10-5~10-4 — / Safety Low ionic conductivity 34
PEO-PTEC-LiTFSI 0.39 / 1~5 V / No electrolyte leakage Low voltage, Compatibility 89
PEO/LiTFSI/MMT 0.45 / 1~4 V 42 Low cost / 29
(PEO-PMMA)-LiClO4 >0.98 / 0~5 V / Excellent processability / 90
Ceramic Li4.08Zn0.04Si0.96O4 0.92 10-4~10-2 1~5.8 V / High ionic conductivity High interfacial Impedance 91
Li9.54Si1.74P1.44S11.7Cl0.3 / / 0.2~5 V 24.6 Preventing LiPSs shuttling / 61
Li7P2.9S10.85Mo0.01 / / 0.5~5 V 22.7 / High cost 86
Li7P2.9Mn0.1S10.7I0.3 / / 0.2~5 V 20.8 Wide electrochem. window Sensitive to moisture11
Li11AlP2S12 ~1 / 0.5~5 V 25.4 / / 55
Composite FDE-LAGP 0.83 10-4~10-3 / / l Preventing LiPSs shuttling Limited capacity 13
PEO-20%LAGP 0.378 / 2.5~6 V / / / 75
LPS-PEO-LiClO4 / / 0.2~5 V 24.43 Suppressing Li dendrite / 77
P(VdF-HFP)/LLZO 0.82 / 0~5 V / / / 92
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