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Progress in Chemistry 2019, Vol. 31 Issue (5): 699-713 DOI: 10.7536/PC180815 Previous Articles   Next Articles

Special Issue: 锂离子电池

Electrolyte Additives for Interfacial Modification of Cathodes in Lithium-Ion Battery

Zhimin Jiang1, Li Wang2, Min Shen1, Huichuang Chen1, Guoqiang Ma1,**(), Xiangming He2,**()   

  1. 1. Zhejiang Chemical Industry Research Institute Co. Ltd., Hangzhou 310023, China
    2. Institute of Nuclear & New Energy Technology, Tsinghua University, Beijing 100084, China
  • Received: Online: Published:
  • Contact: Guoqiang Ma, Xiangming He
  • About author:
    ** E-mail: (Guoqiang Ma);
    (Xiangming He)
  • Supported by:
    Ministry of Science and Technology of China(2016YFE0102200); National Natural Science Foundation of China(U1564205)
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Increasing the voltage is one of the important ways to improve the energy density of lithium ion batteries. For example, LiNi0.5Mn1.5O4 (4.7 V), LiNiPO4(5.1 V) and lithium-rich manganese-based materials exhibit high energy density and low cost at high charge cut-off voltage, showing good application prospects. In addition, increasing the charge cut-off voltage of LiCoO2 and NMC battery systems is a simple and effective approach to increase the energy density. However, when the charge cut-off voltage is increased, not only the electrolyte will be oxidatively decomposed at the cathode /electrolyte interface, but also the dissolution of the metal cation from the cathode materials will be accelerated. These are the main causes for the decreased cycle stability and safety. The electrolyte additives can be used for modifying positive electrode interfaces, thus passivating the cathode/electrolyte interface and inhibiting the decomposition of the electrolyte. Moreover, the modified electrolyte can effectively suppress the destruction of the cathode structure. Based on the molecular structure of the additives, the related research results of additives such as sulfonate ester, boric acid ester, phosphate ester, fluorocarbonate, nitrile, anhydride and lithium salt at the positive electrode interface are introduced in this paper. The action mechanisms of different additives are explained and generalized. Furthermore, the combination technology of additives for different batteries are introduced. At last, the development of new electrolyte additives for cathode/electrolyte interface modification are discussed.

Key words: lithium-ion battery, electrolyte, additives, high voltage
Fig. 1 Structures of additives for cathodes containing sulfur, phosphorus and boron groups
Fig. 2 Structures of additives for cathodes containing fluorine, nitrile groups
Fig. 3 Floating test of F-EMC solvent mixed with EC, TFPC, FEC, and TFP-PC-E at 1∶1 ratio[15]
Fig. 4 The schematic for the surface modification mechanism of the HTN additive on the cathode[63]
Fig. 5 Comparison of electrochemical behaviors of a LNM/LTO cell with and without GA as electrolyte additive[65]
Fig. 6 Structures of additives for cathode of Lithium salt type and others
Scheme. 1 Possible mechanism for the EC decomposition[84]
Table 1 The interface modification on the cathode of different ectrolyte additive and the different performance behavior to batteries
Electrolyte additive Oxidation potential
(V vs. Li+/Li)		 Additive effect ref
Main action mechanism Interface film component Reported battery chemistry and the mechanism of the additives
FEC 6.44(PF6-) Film formation PEO-like polymer, carbonate LiNi0.5Mn1.5O4/graphite: Participate in the formation of protective surface film on cathode; enhance voltage stability at elevated temperature. 15
FEMC 6.26(PF6-) Film formation Metal fluorides, C-F containing species LiNi0.5Mn1.5O4/Li and LiNi0.5Mn1.5O4/Li4Ti5O12: Increase oxidation stsbility in high-voltage; enhance cycling performance. 15
VC 4.85[11] Film formation Ploy(VC) LiCoO2/Li: Form effective passivation layers at the surface of both electrodes; not suitable for the condition of high voltage. 11
ADN 6.9[72] Metal ions absorbing -CN
containing species		 LiCoO2/MCMB: Improve resistance to aluminum; form a stable solid electrolyte interface especially to cathode of LiCoO2. 72
SUN 6.8[72] Metal ions absorbing -CN
containing species		 Li[Li0.2Mn0.56Ni0.16Co0.08]O2/Li: Form a more dense and stabe interface; suppress the decomposition of LiPF6,EC and DMC; enhance capacity performance. 72
BP 4.5[73] Overcharge protection Oligomers having 6-12 benzene rings LiCoO2/graphite: Have lower oxidation potential than solvents; form a thick interfacial film on cathode. 73
HFiP 4.2[74] Film formation CF3-,CF3-CR2- species Li[Li0.2Mn0.56Ni0.16Co0.08]O2/Li: Form a more stable SEI layer; have more stable solid electrolyte impedance and smaller charge transfer resistance. 74
TMSP 4.1[75] Film formation and electrolyte stabilizer Si-O,P-O species LiNi0.5Mn1.5O4/graphite: Alleviate the decomposition of LiPF6 by hydrolysis; eliminate HF promoting Mn/Ni dissolution from the cathode. 75
TMSB 3.76[48] Film formation and electrolyte stabilizer Si-O,B-O species LiMn2O4/Li: Show excellent capacity retention at high temperature; reduce the content of HF. 48
MMDS 4.6[76] Film formation Li2SO3,ROSO2Li,
sulfide component		 LiNi0.5Co0.2Mn0.3O2/graphite: Increase capacity retention; improve the conductivity of CEI; suppress the solvent decompdsition at high voltage. 76
SA 4.4[64] Film formation Hydrocarbons,Li2CO3 LiNi0.5Mn1.5O4/Li: Improve high voltage stability; form a modified protective layer. 64
TB 4.3[50] Film formation and electrolyte stabilizer Metal oxide,
B-O species		 LiNi1/3Co1/3Mn1/3O2/Li: Improve cyclic stability and rate
capability; form a stable and low impedance film.		 50
LiBOB 4.2[74] Film formation and electrolyte stabilizer Li oxalate,
oxalate species		 LiNi0.5Mn1.5O4/Li: React with water traces and suppress the formation of POF3; improve high voltage and high temperature stability. 74
LiDFOB 4.35[77] Film formation and electrolyte stabilizer B containing polycarbonate Li1.2Ni0.15Mn0.55Co0.1O2/ Li: Reduces both cell capacity loss and impedance rise; inhibits electrolyte oxidation; reduces dissolution of metal ions. 77
Scheme. 2 Schematic representation of possible mechanisms for electrochemical oxidative decomposition of TMSP[11]
Scheme. 3 Main possible VC degradation products:(A)radical polymer,(B)linear polymer[87]
Scheme. 4 Electrochemical oxidative decomposition of DFDEC and its further reaction with EC to form a stable SEI[89]
Scheme. 5 Proposed mechanisms for the functions of phosphite-based additives for the HF removal[42]
Scheme. 6 Proposed mechanisms for the LiBOB additive for improvement in electrochemical performance of high-voltage cathode[94]
Scheme. 7 Proposed reaction mechanisms of BP and CHB[97]
Scheme. 8 Proposed mechanisms for the functions of nitrile-based additives for the HF removal[61]
Fig. 7 Effects of nitriles protecting cathode surface from electrolyte(a) nitrile-absent electrolyte and nitrile-present electrolytes of(b) long-chain nitriles and(c) short-chain nitriles[102]
Fig. 8 Optimized structure of EC, EMC, TMSB and TMSP with PF6- and the calculated oxidation potential(vs. Li/Li+)[106]
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