Effect of Microstructure on Chemo-Mechanical Damage Evolution in Aluminum Foil Anodes for Lithium-Ion Batteries

Abstract

Aluminum-based foil anodes could enable lithium-ion batteries with high energy density comparable to silicon and lithium metal. However, mechanical pulverization and lithium trapping within aluminum tend to cause capacity fading. The complex interplay between these damage modes is not well understood, as well as the role of microstructure on reaction front evolution. Here, we investigate aluminum foils with different compositions and processing conditions to understand how microstructure influences chemo-mechanical degradation. Backscattered electron imaging of ion-milled foil cross sections is used to visualize reaction front evolution and chemo-mechanical degradation. We find that the shape of the reaction front during lithiation is strongly affected by foil composition, defect distribution, and grain size, which, in turn, affects the evolution of chemo-mechanical damage within the foils. Furthermore, a key finding is that the extent of fracture upon delithiation is inversely related to lithium trapping, with foil compositions that exhibit uniform lithiation, and therefore, less fracturing showing greater lithium trapping. Nonreactive precipitate inclusions within alloy foils are also found to induce void formation. This work shows that material design strategies designed to overcome the inverse fracture-lithium trapping relationship could be useful for improving performance.