基于锂盐的新型锂电池电解质研究进展

doi:10.15541/jim20170523

无机材料学报 ›› 2018, Vol. 33 ›› Issue (7): 699-710.DOI: 10.15541/jim20170523 CSTR: 32189.14.10.15541/jim20170523

所属专题：离子电池材料

• • 下一篇

基于锂盐的新型锂电池电解质研究进展

马国强^1,2, 蒋志敏², 陈慧闯², 王莉¹, 董经博², 张建君², 徐卫国², 何向明¹

1. 清华大学核能与新能源技术研究院, 北京市精细陶瓷实验室, 北京 100864;
2. 浙江省化工研究院有限公司, 杭州 310023

收稿日期:2017-11-06 修回日期:2018-01-16 出版日期:2018-07-10 网络出版日期:2018-06-19
作者简介:马国强(1986-), 男, 博士. E-mail: maguoqiang@sinochem.com
基金资助:
国家自然科学基金重大项目(U1564205);中国科技部项目(2016YFE0102200);中国博士后科学基金(2016M590550);浙江省科技厅项目(2016F50051);National Natural Science Foundation of China (U1564205);Ministry of Science and Technology of China (2016YFE0102200);China Postdoctoral Science Foundation (2016M590550);Zhejiang Province Research Institutes Special Fund (2016F50051)

Research Process on Novel Electrolyte of Lithium-ion Battery Based on Lithium Salts

MA Guo-Qiang^1,2, JIANG Zhi-Min², CHEN Hui-Chuang², WANG Li¹, DONG Jing-Bo², ZHANG Jian-Jun², XU Wei-Guo², HE Xiang-Ming¹

1. Beijing Key Lab of Fine Ceramics, Institute of Nuclear & New Energy Technology, Tsinghua University, Beijing 100864, China;
2. Zhejiang Chemical Industry Research Institute Co. Ltd., Hangzhou 310023, China

Received:2017-11-06 Revised:2018-01-16 Published:2018-07-10 Online:2018-06-19
About author:MA Guo-Qiang. E-mail: maguoqiang@sinochem.com

摘要/Abstract

摘要：

随着新能源汽车、可携带式电源和储能等领域的快速发展, 人们对锂电池性能提出了更高的要求, 高性能锂离子电池的重要性日益突出。电解质是锂离子电池的重要组成部分, 对于电池的输出电压、倍率性能、适用温度范围、循环性能和安全性能等有着重要的影响。而锂盐作为液体电解质(电解液)的关键组分, 是决定电解液性能的重要因素。电解液中不同种类的锂盐及其在溶液中不同的溶剂化状态, 会对电极/电解液界面的成膜性能和锂离子的迁移行为等产生重要影响, 进而显著影响电解液的电化学性能。本文介绍了近年来新型电解质锂盐的性质特点和在不同种类电池中的应用。同时, 单一的锂盐不能完全满足锂电池对电解液的要求, 因而人们尝试采用复合锂盐使功能更完善, 催生了多盐体系电解液。多盐体系电解液在拓宽电池工作温度、抑制金属离子溶出和提高倍率性能等方面表现出明显优势。同时, 借助于浓度的提升改变锂离子的溶剂化结构, 研究人员提出了高浓度电解液。高浓度电解液在防止石墨剥离、拓宽电解液电化学窗口、抑制铝箔腐蚀和提高金属锂沉积/溶出性能等方面具有明显优势。并且, 本文重点讨论了这两种电解液对电池性能提升的机理。最后, 对锂盐基电解液尤其是这两类新型电解液的发展趋势和应用前景进行了展望。

关键词: 电解质, 锂盐, 多盐电解液, 高浓度电解液, 综述

Abstract:

With the development of electric vehicles, portable applications and energy storage systems, high-performance lithium-ion batteries are urgently demanded, and the corresponding research becomes much more important. Electrolyte is one of the indispensable components for lithium-ion battery, resulting in a significant impact on the rate performance, temperature range, cycling performance, safety issue and so on. Lithium salt as the key component, is an important factor dominating the performance of the electrolyte. Various lithium salts and their solvation structures in the electrolyte evidently affect the quality of SEI layer derived from electrolytes and lithium ion migration behavior, leading to completely different electrochemical properties. The characteristics of different novel lithium salts are introduced in detail. Furthermore, the fact that a single lithium salt can’t meet all the required performance propels to design the high performance electrolyte with multi-salts. This electrolyte shows a series of advantages in expanding the working temperature range, suppressing the metal ion dissolution and improving the rate performance. Simultaneously, based on tuning the solvation structure of Li⁺ by increasing the concentration, a novel concentrated electrolyte is introduced, displaying the advantages such as the suppressed graphite peeling, the expanded electrochemical window, the suppressed Al corrosion, the improved metallic lithium plating/stripping and so on. Furthermore, detail discussion focuses on the mechanisms for the enhanced performance of the two excellent electrolytes. Finally, development tendency and application prospect of lithium-salt based electrolytes, especially these two novel electrolytes are discussed.

Key words: electrolyte, lithium salts, multi-salts electrolyte, concentrated electrolyte, review

中图分类号:

TQ174

马国强, 蒋志敏, 陈慧闯, 王莉, 董经博, 张建君, 徐卫国, 何向明. 基于锂盐的新型锂电池电解质研究进展[J]. 无机材料学报, 2018, 33(7): 699-710.

MA Guo-Qiang, JIANG Zhi-Min, CHEN Hui-Chuang, WANG Li, DONG Jing-Bo, ZHANG Jian-Jun, XU Wei-Guo, HE Xiang-Ming. Research Process on Novel Electrolyte of Lithium-ion Battery Based on Lithium Salts[J]. Journal of Inorganic Materials, 2018, 33(7): 699-710.

图/表 11

表1 一些锂盐的性质

Table 1 Properties of some lithium salts

Lithium salt	Ionic conductivity (Solvent)/(mS∙cm^-1)	Oxidation potential(Solvent and working electrode)/V (vs. Li/Li⁺)	Al- corrosion	Melting point/℃	Initial decomposition temperature/℃
LiPF₆	10.8 (EC : DMC=1 : 1^b)^[32]	>5.1 (EC : DMC=1 : 1^b, Li_l-_xMn₂O₄)^[34]	N	200^[38]	125^[40]
LiClO₄	10.1 (EC : DMC=1 : 1^a)^[32]	>5.1 (EC : DMC=1 : 1^b, Li_l-_xMn₂O₄)^[34]	N	236^[38]	450^[41]
LiBF₄	4.9 (EC : DMC=1 : 1^b)^[32]	>5.1 (EC : DMC=1 : 1^b, Li_l-_xMn₂O₄)^[34]	N	293-300^[38]	175^[40]
LiTFSI	9 (EC : DMC=1 : 1^b)^[32]	4.35 (EC : DMC=1 : 1^b, Li_l-_xMn₂O₄)^[34]	Y	234^[39]	360^[14]
LiFSI	9.73 (EC : EMC=3 : 7^a)^[33]	5.6 (EC : DMC=1 : 1^a, Pt)^[35]	Y	135^[33]	200^[33]
LiBOB	14.9 (DME)^[32]	4.6 (PC : EC : DEC=1 : 1 : 1^a, Pt)^[36]	N	>300^[38]	275^[40]
LiDFOB	8.58 (EC : DMC=1 : 1^a)^[32]	>6 (PC : EC : EMC=1 : 1 : 3^a, Al)^[37]	N	265-271^[38]	200^[40]
LiTDI	6.7 (EC : DMC=1 : 1^b)^[32]	>4.5 (EC: DMC1 : 1^b, Pt)^[31]	N	-	285^[31]

图1 锂离子电池工作原理图[16]

Fig. 1 The working mechanism of lithium-ion battery[16]

图2 Li+溶剂化合物从电解液迁移到石墨层间的过程及相应的阻抗图[43]

Fig. 2 Schematic description of a solvated lithium ion’s journey from solution bulk to grapheneinterior, and the impedance components associated with these steps[43](a) Conventional model; (b) Improved model

图3 石墨/Li半电池在不同倍率下的放电比容量[49]

Fig. 3 Rate capabilities of graphite/Li half cells at various discharge rates[49]

图4 LiTFSI和LiBOB在多盐体系电解液中的作用[56]

Fig. 4 Schematic illustration of the effects of LiTFSI and LiBOB in dual-salt electrolyte[56]

图5 Li+溶剂化合物共嵌导致石墨层的剥离[2]

Fig. 5 The exfoliation of graphite layers caused by Li+-solvent co-intercalation[2]

图6 低浓度和高浓度电解液中SEI膜的主要成分[72]

Fig. 6 The main components of SEI in dilute and concentrated electrolytes[72]

图7 石墨/Li金属半电池在两种电解液中不同充放电倍率下的可逆容量[68]

Fig. 7 Reversible capacity of a natural graphite/Li half cell with two electrolytes at various C-rates[68]

图8 不同浓度电解液中LiTFSI锂盐的分解机理和LiF电解质膜的形成机理(a)1.0 mol/L LiTFSI和(b)1.8 mol/L LiTFSI[73]

Fig. 8 Mechanism for LiTFSI decomposition and formation of LiF film in (a) 1.0 mol/L LiTFSI and (b) 1.8 mol/L LiTFSI[73]

图9 (a)稀浓度和高浓度电解液中不同的Li+溶剂化作用形式(SSIPs、CIPs和 AGGs)(b)稀浓度和(c)高浓度电解液中电极表面发生的界面反应[78]

Fig. 9 (a) Representative Li+ cation solvate species (SSIPs, CIPs and AGGs) in dilute and concentrated electrolytes. Schematic illustration of the electrolyte reduction mechanism at the electrode/electrolyte interface in (b) dilute and (c) concentrated electrolytes[78]

图10 Li+溶剂化结构模型和通过DFT-MD模拟计算得到的PDOS值(a)稀浓度电解液(b)高浓度电解液[78]

Fig. 10 Supercells used and projected density of states (PDOS) obtained in quantum mechanical DFT-MD simulations on non-aqueous (a) dilute (0.4 mol/L) and (b) superconcentrated (4.2 mol/L) LiTFSA/AN solutions[78]

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基于锂盐的新型锂电池电解质研究进展

Research Process on Novel Electrolyte of Lithium-ion Battery Based on Lithium Salts

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