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Progress in Chemistry 2020, Vol. 32 Issue (6): 761-791 DOI: 10.7536/PC191116 Previous Articles   Next Articles

Special Issue: 电化学有机合成; 锂离子电池

• Review •

Research Progress on Diagnosis of Electrochemical Impedance Spectroscopy in Lithium Ion Batteries

Quanchao Zhuang1,**(), Zi Yang1, Lei Zhang1, Yanhua Cui2,**()   

  1. 1. School of Materials and Physics, China University of Mining and Technology, Xuzhou 221116, China
    2. Institute of Electronic Engineering, China Academy of Engineering Physics, Mianyang 621900, China
  • Received: Revised: Online: Published:
  • Contact: Quanchao Zhuang, Yanhua Cui
  • Supported by:
    the National Natural Science Foundation of China(U1730136); the Fundamental Research Funds for the Central Universities(2017XKQY062)
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Electrochemical impedance spectroscopy (EIS) is one of the most powerful experimental methods to study electrochemical systems, and has been extensively used in the analysis of lithium battery systems, especially to determine kinetic and transport parameters, understand reaction mechanisms, and to study degradation effects in past two decades. In this paper, the electrode polarization process in lithium ion batteries which includes three basic physical and chemical processes, namely, electronic transport process, ionic transport process and electrochemical reaction process, is briefly described, and the EIS characteristics of each transport and reaction stage of the three basic physical and chemical processes are discussed, especially the mechanism of inductance formation and contact impedance is expounded in detail. Moreover, porous electrode theory and its application in lithium ion batteries are reviewed, and emphasis is put upon the principle and method of numerical simulation of impedance with physics-based lithium-ion batteries models. Furthermore, the typical EIS characteristics and the attribution of each time constant of the electrode materials for lithium ion batteries such as graphite, silicon, simple binary transition metal oxides, LiCoO2, spinel LiMn2O4, LiFePO4, spinel Li4Ti5O12 and transition metal oxides are also discussed. Finally, the challenges currently faced by EIS are identified and possible directions and approaches in addressing these challenges are suggested.

Contents

1 Introduction
2 Theoretical basis for EIS analysis of lithium ion batteries

2.1 Schottky contact impedance

2.2 The mechanism of inductance formation

2.3 Porous electrode theory and numerical simulation of impedance and their applications in lithium ion batteries

3 The EIS characteristics of lithium ion battery electrodes

3.1 The EIS characteristics of lithium ion battery anode

3.2 The EIS characteristics of lithium ion battery cathode

4 Conclusion and prospect
Key words: lithium ion battery, electrochemical impedance spectroscopy, porous electrode, numerical simulation
Fig. 1 Schematic presentation of model for the physical mechanism of lithium ion insertion
Fig. 2 Variations of impedance spectra of LiCoO2 electrode with the polarization potential in the first delithiation[40]
Fig. 3 Pictorial representation model for the SEI film growth and the concentration cell[40]
Fig. 4 Schematic diagram of intercalation particle, with a detailed picture of the particle-film and film-solution interface and an equivalent-circuit diagram of the interfaces[54]
Fig. 5 Schematic diagram showing the construction of a porous electrode consisting of spherical particles[54]
Fig. 6 Schematic diagram showing the differential flow of current in a porous electrode in which current can flow in both the solid and solution phases[54]
Fig. 7 Nyquist plots of the graphite electrode at various potentials from 3.0 to 0.1 V during the first lithium-ion insertion[64]
Fig. 8 Schematic view of two general models of the porous electrode[64]
Fig. 9 Model of a cylindrical pore; gray area is not conductive. I: axial current flowing to pore, j: local current flowing to pore walls
Fig. 10 Complex plane plot of impedance of single pore
Fig. 11 Schematic diagram of uniform transmission line model. Uniform transmission line representing impedance of flooded ideally polarized porous electrode; rs and cdl are the solution resistance and double-layer capacitance, respectively, of a small element of the pore length
Fig. 12 Transmission line for the capacitive porous electrode with the resistance of the solution in pores, rs, and of the electrode material, re
Fig. 13 Nyquist plots of graphite electrodes with thickness of 0.1, 0.2, 0.4 and 0.6 mm in the first discharge process[77]
Fig. 14 Nyquist plots of the LiNi1/3Co1/3Mn1/3O2 cathode during the first charge process in 1 M LiPF6-EC:EMC electrolyte with 2%DTD+1%MMDS[77]
Fig. 15 Nyquist diagram of the graphite electrode in the first lithiation[81,82]
Fig. 16 Nyquist diagram of the Si/C electrode in the first lithiation[91]
Fig. 17 Nyquist plots of the α-Fe2O3/C composite electrode at various polarization potentials during the first discharge process[99]
Fig. 18 Nyquist diagram of LixNi0.75Co0.25O2 electrode[119]
Fig. 19 Nyquist spectrum and fitting diagram of LiCoO2 electrode at various potentials from 3.6 to 4.3 V in the first delithiation[123]
Fig. 20 Nyquist plots of the spinel LiMn2O4 electrode at various potentials from 3.5 to 4.3 V during the first delithiation at 10°C[129]
Fig. 21 Nyquist plots of the LiFePO4 electrode with 50 weight percent (wt%) graphite as conductive agent at various potentials from 3.3 to 4.2 V during the first delithiation[141]
Fig. 22 Nyquist plots of the Li4Ti5O12 electrode at a series of potentials from 2.8 to 1.0 V in the first lithiation process [146]
Fig. 23 Nyquist plots of the NiF2/C electrode at various potentials from 3.15 to 1.2 V during the first discharge process[31]
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