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Progress in Chemistry 2021, Vol. 33 Issue (5): 855-867 DOI: 10.7536/PC200634 Previous Articles   Next Articles

Special Issue: 锂离子电池

• Original article •

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: Revised: Online: Published:
  • 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)
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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
Fig. 1 The molecular structures of some fluorinated solvents
Fig. 2 The molecular structures of some nitrile-based solvents
Fig. 3 The molecular structures of some sulfone-based solvents
Fig. 4 The molecular structures of some ionic liquids
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
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]
Fig. 6 The molecular structures of some phosphorous additives
Fig. 7 The molecular structures of some boronated additives
Fig. 8 The molecular structures of some benzene and heterocyclic additives
Fig. 9 The molecular structure of some additives
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
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
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]
Fig. 11 Solvent phase reaction energies(ΔG in kcal·mol-1) of TMSB and TMSB+ with a LiF molecule[97]
Fig. 12 Solvent phase reaction energies of TPP with a HF molecule[62]
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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