Spatiotemporal Changes of the Solid Electrolyte Interphase in Lithium‐Ion Batteries Detected by Scanning Electrochemical Microscopy

The solid electrolyte interphase (SEI) in lithium-ion batteries separates the highly reductive lithiated graphite from reducible electrolyte components. It is critical for the performance, durability, and safe operation of batteries. In situ imaging of the SEI is demonstrated using the feedback mode of scanning electrochemical microscopy (SECM) with 2,5-di-tert-butyl-1,4-dimethoxy benzene as mediator. The formation of the SEI is indicated by a decrease of the mediator regeneration rate. Prolonged imaging of the same region revealed fluctuation of the passivating properties on time scales between 2 min and 20 h with an inhomogeneous distribution over the sample. The implications of the approach for in situ assessment of local SEI properties on graphite electrodes are discussed with respect to studying the influence of mechanical stress on SEI reliability and the mode of action of electrolyte additives aiming at improving SEI properties.