Dynamics of Solid‐Electrolyte Interphase Formation on Silicon Electrodes Revealed by Combinatorial Electrochemical Screening

Revealing how formation protocols influence the properties of solid-electrolyte interphase (SEI) on Si electrodes is key to developing next generation Li-ion batteries. SEI understanding is, however, limited by low-throughput nature conventional characterisation techniques. Herein, correlative scanning electrochemical cell microscopy (SECCM) and shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) are used for combinatorial screening under a broad experimental space (20 sets different conditions with several repeats). This novel approach reveals heterogeneous dynamics chemical composition electrodes, which evolve in characteristic manner as function cycle number. Correlative SECCM/SHINERS has potential screen thousands candidate experiments variety battery materials accelerate optimization methods, bottleneck manufacturing.