Dynamics of the Morphological Degradation of Si‐Based Anodes for Li‐Ion Batteries Characterized by In Situ Synchrotron X‐Ray Tomography

Abstract The alloying reaction of silicon with lithium in negative electrodes for lithium‐ion batteries causes brutal morphological changes that severely degrade their cyclability. In this study, the dynamics of their expansion and contraction, of their cracking in the bulk and of their debonding at the interface with the current collector are visualized by in situ synchrotron X‐ray computed tomography and quantified from appropriate 3D imaging analyses. Two electrodes made with same silicon material having reasonable particle size distribution from an applied point of view are compared: one fabricated according to a standard process and the other one prepared with a maturation step, which consists in storing the electrode in a humid atmosphere for a few days before drying and cell assembly. All morphological degradations are significantly restrained for the matured electrode, confirming the great efficiency of this maturation step to produce a more ductile and resilient electrode architecture, which is at the origin of the major improvement in their cyclability.