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The electrochemical impedance spectroscopy (EIS) technique has been widely used for analysing lithium battery systems, especially to determine kinetic and transport parameters, understand reaction mechanisms, and study capacity fade mechanisms. In this work, the initial charge-discharge process of LiCoO2@LiNbO3/Li10GeP2S12/Li (LLCO/LGPS/Li) and LiNi0.5Co0.2Mn0.3O2@LiNbO3/Li10GeP2S12/Li (LNCM523/LGPS/Li) batteries at different potentials was systematically investigated by EIS. During the lithium-ion insertion-removal process, the Nyquist plots of both LLCO/LGPS/Li and LNCM523/LGPS/Li batteries are composed of three parts, namely, two semicircles and an inclined line, which can be attributed to the interfacial impedance between the solid electrolyte and electrode, the charge transfer process, and the solid-state diffusion of the lithium-ion in the cathode with decreasing frequency, respectively. A proper equivalent circuit is proposed to fit the experimental EIS data and the variations in the interfacial resistance (Rif) between the solid electrolytes (SEs) and electrode. The charge transfer resistance (Rct) along with the increase or decrease in the electrode polarization potential is quantitatively analysed in detail. Based on the experimental results, it has been revealed that, the increase in Rif between the solid electrolyte and electrode may cause the capacity fade of all-solid-state batteries during charge-discharge.

Electrochemical Impedance Spectroscopy Study on Using Li10GeP2S12 Electrolyte for All-Solid-State Lithium Batteries