锂离子电池固体电解质的研究与进展

doi:10.3969/j.issn.1674-8484.2020.04.001

汽车安全与节能学报 ›› 2020, Vol. 11 ›› Issue (4): 415-427.DOI: 10.3969/j.issn.1674-8484.2020.04.001

• 综述与展望 • 下一篇

锂离子电池固体电解质的研究与进展

穆道斌¹(), 谢慧琳¹, 吴伯荣¹^,²^,^*()

1.北京理工大学能源与环境材料系,北京100081,中国
2.北京市电动汽车协同创新中心,北京100081,中国

收稿日期:2020-09-16 出版日期:2020-12-30 发布日期:2021-01-04
通讯作者: 吴伯荣
作者简介:*吴伯荣（1964—）,男(汉),江西,教授。E-mail:Wubr@bit.edu.cn。吴伯荣教授工学博士、北京理工大学教授、博士生导师。担任中国汽车工程学会电动汽车分会副主任委员,动力电池北京市高等学校工程技术研究中心副主任及技术委员会委员,中国绿色能源产业技术创新战略联盟副秘书长、技术委员会副主任等职务。主要研究方向为新型锂离子电池、金属锂电池及全固态电池、超级电容器及相关关键材料等。发表SCI论文百余篇,先后获部级科技进步一等奖1项、二等奖6项、三等奖1项等奖励;获国家授权发明专利20余项,出版专著（合著）2部、译著3部。
穆道斌（1968—）,男（汉）,北京,教授。E-mail: mudb@bit.edu.cn。穆道斌教授工学博士、北京理工大学教授、博士生导师。主要研究方向为新能源材料及器件、应用电化学等,涉及二次电池关键材料设计研制、电池反应机制、理论计算及仿真研究等。主持国家自然科学基金等多项研究项目,已发表70余篇SCI论文及获多项国家发明专利，出版译著2部。
Prof. MU Daobin PhD in engineering. He is a professor and a doctoral adviser of the Beijing Institute of Technology. His research interests focus on such areas as energy materials and devices, applied electrochemistry, etc., involving the design and development of key materials for secondary batteries, battery reaction mechanism, theoretical calculation and simulation research, etc. He has presided over a number of projects such as those funded by the National Natural Science Foundation of China. He has published more than 70 SCI papers and authorized multiple national invention patents, and has also translated 2 books
基金资助:
国家重点研发计划(2017YFB0102000);国家自然基金项目(52072036);“十三五”装备预研项目(41421040202);上海航天科技创新基金项目(SAST2018-114)

Research and development of solid electrolytes for lithium ion batteries

MU Daobin¹(), XIE Huilin¹, WU Borong¹^,²^,^*()

1. Department of Energy & Environmental Materials, Beijing Institute of Technology, Beijing 10081, China
2. Collaborative Innovation Center of Electric Vehicles in Beijing, Beijing 10081, China

Received:2020-09-16 Online:2020-12-30 Published:2021-01-04
Contact: WU Borong

摘要/Abstract

摘要：

固态锂离子电池因具备能量密度高、安全性能好等优点,已经成为了未来动力电池的主流发展方向。该文详细梳理了固态锂离子电池的组成和特性以及其核心组成部分─固体电解质的类型与研究进展;简述了当前固态锂离子电池的研发现状,重点阐述了石榴石型锂镧锆氧（Li₇La₃Zr₂O₁₂）基固体电解质在改善锂离子电导率以及界面调控的研究。该类型固体电解质凭借良好的室温离子电导率、优异的金属锂复合相容性,以及在应用环境下可靠稳定的突出特性,有望成为未来全固态锂离子动力电池的重要组成单元。指出固体电解质材料的研发势将会对未来固态锂离子动力电池乃至电动汽车领域的发展提供巨大的推力,前景广阔。

关键词: 电动汽车, 固态锂离子电池, 固体电解质, 锂镧锆氧（Li₇La₃Zr₂O₁₂）, 安全性

Abstract:

Solid-state lithium-ion batteries have become the promising development direction of power batteries due to their high energy density and excellent safety performance. This paper reviews the component and characteristics of solid-state lithium-ion batteries in detail, as well as the types and research progress of solid electrolytes. Moreover, this review also briefly describes the current status of solid-state lithium-ion batteries, and focuses on the garnet-type lithium lanthanum zirconium oxide (Li₇La₃Zr₂O₁₂-based) solid electrolytes which have outstanding advantages in lithium ion conductivity and interface regulation. As one important component of all-solid lithium ion power batteries, the garnet-type Li₇La₃Zr₂O₁₂-based solid electrolytes have good ionic conductivity at room temperature, excellent metal-lithium interface compatibility, and outstanding stability under application environment. The breakthrough and development of solid electrolytes will inevitably provide a huge thrust for the future development of solid-state lithium-ion power batteries and even electric vehicles.

Key words: electric vehicles, solid state lithium ion batteries, solid electrolytes, lithium lanthanum zirconium oxide (Li₇La₃Zr₂O₁₂), safety

中图分类号:

TQ152

穆道斌, 谢慧琳, 吴伯荣. 锂离子电池固体电解质的研究与进展[J]. 汽车安全与节能学报, 2020, 11(4): 415-427.

MU Daobin, XIE Huilin, WU Borong. Research and development of solid electrolytes for lithium ion batteries[J]. Journal of Automotive Safety and Energy, 2020, 11(4): 415-427.

图/表 15

图1 锂离子电池和固态电池结构的对比示意图[17]

图2 不同电解质的性能雷达图[25]

企业及研究机构	固体电解质	离子电导率/ (S·cm^-1)	性能值/ (Wh·kg^-1)	备注
Bollore	PEO + Li盐	10^-7~10^-5	100	已应用于商业化汽车
宁德时代	PEO +Li盐	10^-7~10^-5	100	制备了安全性能好的实验产品
台湾辉能	非薄膜氧化物	10^-6~10^-3	800 (2020年)	在消费电池领域已商用
Quantumscape	非薄膜氧化物	10^-6~10^-3	400	准备应用于大众汽车
清陶能源	非薄膜氧化物	10^-6~10^-4	400	固态锂电池产线正式投产
Sakti3	薄膜型氧化物	10^-6~10^-3	1000	应用于戴森N526汽车
丰田	硫化物	10^-7~10^-2	400	电动汽车将于东京奥运会亮相
Sony	硫化物	10^-7~10^-2	500	面向移动设备和电动车辆研发

表1 近年来固态锂离子电池的研究进展

图3 立方Li7La3Zr2O12的晶体结构[40]

图4 四方相和立方相的锂的占据情况示意图

图5 迁移机制示意图[45]

图6 Li+在立方晶格中的迁移路径[49] a. Li+从Li2O6到Li1O4再到Li2O6的迁移路径;b. 锂离子运输路径的瓶颈尺寸(红色虚线表示共边长度增加,蓝色虚线表示共边长度减少)

图7 不同位置晶界结构[62]

图8 晶界对电解质性能的示意图[65]

图9 LLZTO/LBO复合电解质片的测试结果[68]

图10 利用石墨添加剂合成陶瓷相容的且与LLZO紧密接触锂负极（Li-C复合材料）径[78] a. 在LLZO上沉积纯锂;b.在LLZO上沉积锂—石墨复合材料

图11 三明治C-LLZO-C固体电解质片改性前后界面SEM图像[81]

图12 典型正极材料现有水平和发展潜力[82]

图13 全固态正极/电解质表面处理原理图[87]

图14 电解液LiPF6、LiTFSI分别和LLZTO电解质的接触对比[88]

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锂离子电池固体电解质的研究与进展

Research and development of solid electrolytes for lithium ion batteries

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