Understanding of Lithium-ion battery degradation using multisine-based nonlinear characterization method

The nonlinearity of lithium-ion battery voltage response has been recently gained high attention in battery characterization and health diagnosis. The multisine-based nonlinear characterization method has the potential for development as an expedient on-board technique for analyzing nonlinear responses. Despite this, it remains challenging to analyze the effect of aging degradation on LIB nonlinearity. In this study, the odd random-phase multisine method is performed on fresh and aged three-electrode experimental cells. This allowed for the separation of impedance-related linear approximation and odd or even order nonlinearity toward the full-cell voltage into their respective electrodes. The results demonstrate that, as the LIB degrades, the increase of impedance-related linear approximation estimated by the multisine-based method agrees well with the results of conventional EIS. The variation of nonlinearities is demonstrated in relation to the effect of degradation modes. The multisine-based method presents the advantage of simultaneously capturing impedance-related and nonlinearity information. This makes it become a fast diagnostic method that can be implemented in a BMS to quantify the causes of battery degradation, thereby supporting battery utilization optimization and future battery designs. •A multisine nonlinear characterization method is used to investigate LIB degradation.•A 3-electrode set-up is characterized for individual electrode degradation analysis.•Frequency domain response of individual electrodes is analyzed during cycle aging.•The nonlinearity in LIB voltage is demonstrated to provide degradation information.