Investigation of physico-chemical processes in lithium-ion batteries by deconvolution of electrochemical impedance spectra

The individual physico-chemical processes in lithium-ion batteries namely solid-state diffusion and charge transfer polarization are difficult to be tracked by impedance spectroscopy due to simultaneous contributions from cathode and anode. A deeper understanding of various polarization processes in lithium-ion batteries is important to enhance storage performance and cycle life. In this context, the polarization processes occurring in cylindrical 18650 cells comprising different cathodes against graphite anode (LiNi0.2Mn0.2Co0.6O2 vs. graphite; LiNi0.6Mn0.2Co0.2O2 vs. graphite; LiNi0.8Co0.15Al0.05O2 vs. graphite and LiFePO4 vs. graphite) are investigated by deconvolution of impedance spectra across various states of charge. Further, cathodes and anodes are extracted from the investigated 18650-type cells and tested in half-cells against Li-metal as well as in symmetric cell configurations to understand the contribution of cathode and anode to the full cells of various battery chemistries studied. Except for the LiFePO4 vs. graphite cell, the polarization resistance in graphite of other cells are found to be higher than those of the investigated cathodes, proving that the polarization in lithium-ion battery is largely influenced by the graphitic anode. Furthermore, the charge transfer polarization resistance encountered by the cathodes investigated in this work is found to be a strong function of the states of charge.