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化学进展 2021, Vol. 33 Issue (5): 855-867 DOI: 10.7536/PC200634 前一篇   后一篇

所属专题： 锂离子电池

• 研究论文 •

锂离子电池高压电解液

黄国勇1, 董曦1, 杜建委1, 孙晓华1, 李勃天1, 叶海木1,*()   

  1. 1 中国石油大学(北京) 新能源与材料学院 重质油国家重点实验室 北京 102249
  • 收稿日期:2020-06-10 修回日期:2020-08-24 出版日期:2021-05-20 发布日期:2020-12-22
  • 通讯作者: 叶海木
  • 作者简介:
    * Corresponding author e-mail:
  • 基金资助:
    国家自然科学基金项目(51834008); 北京市自然科学基金项目(2202047); 特种化学电源国家重点实验室开放课题(SKL-ACPS-C-20); 中国石油大学(北京)科研基金(ZX20180416)
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High-Voltage Electrolyte for Lithium-Ion Batteries

Guoyong Huang1, Xi Dong1, Jianwei Du1, Xiaohua Sun1, Botian Li1, Haimu Ye1,*()   

  1. 1 College of New Energy and Materials, State Key Laboratory of Heavy Oil, China University of Petroleum,Beijing 102249, China
  • Received:2020-06-10 Revised:2020-08-24 Online:2021-05-20 Published:2020-12-22
  • Contact: Haimu Ye
  • Supported by:
    National Natural Science Foundation of China(51834008); Beijing Municipal Natural Science Foundation(2202047); Opening Project of State Key Laboratory of Advanced Chemical Power Sources(SKL-ACPS-C-20); Science Foundation of China University of Petroleum, Beijing(ZX20180416)

锂离子电池作为一种绿色可充电电池,具有较高能量密度以及功率密度,是便携式电子产品的首选,并逐渐应用于动力汽车领域。为了更好地满足其应用需求,需要进一步提高当前锂离子电池的能量密度。不同于高压正极材料的快速发展,传统电解液在较高工作电压下容易分解,很大程度上阻碍了高能量密度锂离子电池的商业化应用。作为锂离子电池的重要组分,电解液对其多方面性能均具有重要影响,因此亟需提高电解液的工作电压以解决锂离子电池能量密度较低的问题。本文从新型有机溶剂以及高电压添加剂两方面入手,综述近年来国内外高压电解液的研究进展,介绍理论计算对于设计高压电解液的作用,并对高压电解液的发展及前景做出总结和展望。

关键词： 锂离子电池, 电解液, 溶剂, 添加剂, 理论计算

As a kind of green rechargeable battery with high energy density and power density, lithium-ion batteries are the first choice of portable electronic products and are gradually applied in the field of power vehicles. In order to better meet application requirements, it is necessary to further improve the energy density of current lithium-ion batteries. Different from the rapid development of high-voltage anode materials, traditional electrolyte is easy to decompose under high working voltage, which greatly hinders the commercial application of high energy density lithium-ion batteries. As an important component of lithium-ion batteries, electrolyte has an important impact on performance of lithium-ion batteries in many aspects. Therefore, it is urgent to improve the working voltage of electrolyte to solve the problem of low energy density of lithium-ion batteries. In this paper, the research progress of high-voltage electrolyte at home and abroad in recent years is summarized from two aspects of new organic solvent and high-voltage additive, the effect of theoretical calculation on the design of high-voltage electrolyte is introduced, and the development and prospect of high-voltage electrolyte are summarized and forecast.

Contents

1 Introduction

2 New solvents with wide electrochemical window

2.1 Fluorinated solvents

2.2 Nitrile-based solvents

2.3 Sulfone-based solvents

2.4 Ionic liquids

3 High-voltage electrolyte additives

3.1 Phosphorous additives

3.2 Boronated additives

3.3 Benzene and heterocyclic additives

3.4 Others

4 The effect of theoretical calculation on the preparation of high-voltage electrolyte

5 Conclusion and outlook

Key words: lithium-ion batteries, electrolyte, solvent, additive, theoretical calculation
()
图1 几种氟代溶剂的分子结构
Fig. 1 The molecular structures of some fluorinated solvents
图2 几种腈类溶剂的分子结构
Fig. 2 The molecular structures of some nitrile-based solvents
图3 几种砜类溶剂的分子结构
Fig. 3 The molecular structures of some sulfone-based solvents
图4 几种离子液体的分子结构
Fig. 4 The molecular structures of some ionic liquids
表1 不同高压溶剂的性能
Table 1 Properties of different high-voltage solvents
Solvent Components Oxidation potential Capacity retention rate/% ref
Fluorinated FEC LNMO/MCMB, 1 mol/L LiPF6-FEC/DMC/EMC/HFPM(2∶3∶1∶4, by volume) 5.5 V 82.0(0.5 C, 200 cycles) 17
ETFEC LNMO/Li, 1 mol/L LiPF6-EC/DEC/ETFEC(3∶6∶1, by weight) 6.5 V 90.5(0.2 C, 300 cycles) 21
TTE LNMO/Li,1 mol/L LiPF6-FEC/DMC/EMC/TTE(2∶3∶1∶4, by volume) 5.5 V 98.3(1 C, 200 cycles) 24
Nitrile-based ADN MCMB/LiCoO2, 1 mol/L LiTFSI+0. 1 mol/L LiBOB-ADN/EC(1∶1, by volume) 6.0 V 90.0(C/12, 500 cycles) 29
GLN MCMB/LiCoO2, 1 mol/L LiTFSI+0.1 mol/L LiBOB-GLN/EC(1∶1, by volume) 6.0 V 74.0(C/12, 100 cycles) 30
MGLN LTO/NMC, 1 mol/L LiTFSI-MGLN 4.6 V 98.0(0.5 C, 200 cycles) 31
BN NMC/graphite, 1 mol/L LiPF6-BN/EC(9∶1, by volume) + 3% FEC 4.9 V 95.0(5 C, 110 cycles) 32
Sulfone-based EMS LNMO/Li, 1 mol/L LiPF6-EMS/DMC(1∶1, by weight) 5.9 V 97.8(0.2 C, 100 cycles) 36
SL LNMO/graphite, 3.25 mol/L LiFSI-SL 5.0 V 70.0(0.5 C, 1000 cycles) 41
MESL NMC/Li, 1 mol/L LiTFSI-MESL 4.9 V 43
Ionic liquids N1123TFSI LiMn2O4/Li, 0.25 mol/L LiTFSI-N1123TFSI/EC(8∶2, by volume) 6.0 V 87.0(0.1 C, 40 cycles) 51
PYR13TFSI LNMO/Li, 3 mol/L LiPF6-EC/DEC+25% PYR13TFSI 5.6 V 97.0(1 C, 300 cycles) 52
PYR1(2O2)TFSI LiFePO4/Li, 1.0 mol/L
LiTFSI-PYR1(2O2)TFSI/DMC(8:2, by volume)		 \ 93.0(1 C, 200 cycles) 53
图5 不同添加剂在NMC/石墨电池上的成膜机理及相应负极SEI厚度和成分[58]
Fig. 5 Film formation mechanism of different additives of NMC532/AG cells, and the different thicknesses and components in the corresponding SEI on the anode[58]
图6 几种磷类添加剂的分子结构
Fig. 6 The molecular structures of some phosphorous additives
图7 几种硼类添加剂的分子结构
Fig. 7 The molecular structures of some boronated additives
图8 几种苯环及杂环添加剂的分子结构
Fig. 8 The molecular structures of some benzene and heterocyclic additives
图9 几种添加剂的分子结构
Fig. 9 The molecular structure of some additives
表2 不同高压添加剂的性能
Table 2 Properties of different high-voltage additives
Solvent Components Oxidation potential Capacity retention rate/% ref
Phosphorous TMSP LNMO/MCMB, 1 mol/L LiDFOB-SL + 5 wt% TMSP 5.0 V 80.5(0.5 C, 300 cycles) 61
TPP NMC532/graphite, 1 mol/L LiPF6-EC/EMC(3∶7, wt%) + 1 wt% TPP 6.5 V 58.3(1 C, 400 cycles,55 ℃) 62
TPPO NMC811/graphite, 1 mol/L LiPF6-EC/EMC(3∶7, wt%) + 0.5 wt% TPPO 5.4 V 92.0(0.5 C, 100 cycles) 63
TPFPP LLO/graphite, 1 mol/L LiPF6-EC/EMC(3∶7, wt%) + 0.5 wt% TPFPP 5.4 V 90.6(0.3 C, 200 cycles) 64
Boronated TIB NMC622/Li, 1 mol/L LiPF6-EC/EMC/DEC(1∶1∶1, wt%) + 1 wt% TIB >4.5 V 82.7(1 C, 300 cycles) 68
TMB LiCoO2/Li, 1 mol/L LiPF6-EC/DMC(1∶1, vol%) + 2 wt% TPFPP 5.5 V 81.0(0.1 C, 100 cycles) 69
TPFPB LNMO/Li, 1 mol/L LiPF6-EC/EMC(3∶7, wt%) + 1 wt% TPFPB 5.6 V 90.0(0.5 C, 500 cycles) 70
LiBOB LNMO/Li, 1.3 mol/L LiPF6-EC/EMC/DMC(3∶4∶3, vol%) + 1 wt% LiBOB >4.6 V 78.7(0.5 C, 80 cycles, 60 ℃) 73
LiDFOB LiCoPO4/Li, 1 mol/L LiPF6-EC/PC/EMC(1∶1∶3, vol%) + 5 wt% LiDFOB 4.9 V 69.4(0.1 C, 40 cycles) 82
Benzene
Heterocyclic 		4-ABA Li1.2Ni0.2Mn0.6O2/Li, 1 mol/L LiPF6-EC/DEC(1∶1, vol%) + 0.25 wt% 4-ABA >4.5 V 94.4(0.1 C, 100 cycles) 84
BzTz LiCoO2/graphite, 1 mol/L LiPF6-EC/DMC(3∶7, vol%) + 1 wt% BzTz 5.6 V 74.0(5 C, 100 cycles) 85
3THP LNMO/Li, 1 mol/L LiPF6-EC/DMC(1∶2, vol%) + 0.25 wt% 3THP 4.9 V 91.0(1 C, 350 cycles) 86
Others VC NMC532/graphite, 1 mol/L LiPF6-EC/DMC/PC(1∶3∶1, vol%) + 2 wt% VC 4.7 V 90.7(1 C, 120 cycles) 90
PS Li-rich-NMC/Li, 1 mol/L LiPF6-EC/EMC(1∶1, wt%) + 1 wt% PS 4.6 V 88.4(0.2 C, 240 cycles) 89
SA NMC811/Li, 1 mol/L LiPF6-EC/EMC(3∶7, wt%) + 3 wt% SA 5.6 V 93.8(1 C, 400 cycles) 91
BDTT NMC532/graphite, 1 mol/L LiPF6-EC/EMC(3∶7, vol%) + 1 wt% VC+2wt% BDTT 86.0(0.5 C, 200 cycles) 92
表3 几种溶剂的HOMO与LUMO能级比较[21]
Table 3 HOMO and LUMO values of several solvents[21]
Molecule HOMO(eV) HOMO(eV)
EC -8.47 -0.60
DEC -8.02 -0.42
FEC -8.97 -0.64
ETFEC -8.63 -0.48
DTFEC -9.22 -0.68
图10 (a) 溶剂和添加剂分子以及与锂离子溶剂化的有机分子HOMO能级;(b) 不同配合物的HOMO和LUMO能级与配合BODFP的溶剂分子数的关系[96]
Fig. 10 (a) The calculated HOMO values of solvents and additive molecules and the organic molecules solvated with Li ions;(b) The calculated HOMO and LUMO values of different complexes with the number of solvent molecules coordinating with the BODFP[96]
图11 TMSB和TMSB+与LiF分子的溶剂相反应能(ΔG kcal·mol-1)[97]
Fig. 11 Solvent phase reaction energies(ΔG in kcal·mol-1) of TMSB and TMSB+ with a LiF molecule[97]
图12 TPP与HF分子的溶剂相反应能[62]
Fig. 12 Solvent phase reaction energies of TPP with a HF molecule[62]
表4 各类高压溶剂的优缺点
Table 4 Advantages and disadvantages of various high-voltage solvents
Category Advantage Disadvantage
Fluorinated High oxidation stability, non-flammable, excellent wetting ability with separator High viscosity, unstable at high temperature
Nitrile-based Wide electrochemical window(>8 V), low vapor pressure, high boiling point, high flash point High viscosity, poor wetting ability with separator and cathode
Sulfone-based High oxidation potential(>5.4 V), high dielectric constant, high flash point High viscosity, low ionic conductivity
Ionic liquid High chemical and thermal stability, wide electrochemical window, non-flammable High cost, high viscosity, poor wetting ability with separator and cathode
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锂离子电池高压电解液