Nonlinear Electrochemical Impedance Spectroscopy for Lithium-Ion Battery Model Parameterization

In this work we analyse the local nonlinear electrochemical impedance spectroscopy (NLEIS) response of a lithium-ion battery and estimate model parameters from measured NLEIS data. The analysis assumes single-particle including diffusion lithium within electrode particles asymmetric charge transfer kinetics at their surface. Based on assuming moderately-small excitation amplitude, systematically derive analytical formulae for impedances up to second harmonic response, allowing meaningful interpretation each contribution in terms physical processes nonlinearities model. implications parameterization are explored, structural identifiability parameter estimation using maximum likelihood, with both synthetic experimentally Accurate fits data possible, however inconsistencies fitted timescales suggest that may not be appropriate cells considered. Model validation is also demonstrated by predicting time-domain voltage parameterized shown have excellent agreement time-series (11.1 mV RMSE).