Cell-format-dependent mechanical damage in silicon anodes

Abstract: It is generally believed that silicon-based anodes for Li-ion batteries would benefit from stronger binders, as cyclic volume changes would not disrupt the cohesion of the composite electrode. Here, we put this belief to the proof by testing electrodes containing SiOx particles and an aromatic polyimide binder. We observe that the electrodes can stretch laterally by as much as 6% during the first cycle, indicating that internal stresses are high enough to induce plastic deformation on the copper current collector. Remarkably, no coating delamination is observed. Additional consequences were size-dependent: while pouch-cell-sized electrodes developed wrinkles, coin-cell-sized ones remained mostly smooth. We demonstrate that wrinkling of the current collector damages the electrode coating, inactivating SiOx domains and accelerating capacity fade. This size-dependent performance decay indicates that, in extreme cases, testing outcomes are highly dependent on scale. Novel battery materials may require testing at larger cell formats for complete validation.