Textured Electrodes: Manipulating Built‐In Crystallographic Heterogeneity of Metal Electrodes via Severe Plastic Deformation

Abstract Control of crystallography of metal electrodeposit films has recently emerged as a key to achieving long operating lifetimes in next‐generation batteries. It is reported that the large crystallographic heterogeneity, e.g., broad orientational distribution, that appears characteristic of commercial metal foils, results in rough morphology upon plating/stripping. On this basis, an accumulative roll bonding (ARB) methodology—a severe plastic deformation process—is developed. Zn metal is used as a first example to interrogate the concept. It is demonstrated that the ARB process is highly effective in achieving uniform crystallographic control on macroscopic materials. After the ARB process, the Zn grains exhibit a strong (002) texture (i.e., 002 Zn //ND). The texture transitions from a classical bipolar pattern to a nonclassical unipolar pattern under large nominal strain eliminate the orientational heterogeneity of the foil. The strongly (002)‐textured Zn remarkably improves the plating/stripping performance by nearly two orders of magnitude under practical conditions. The performance improvements are readily scaled to achieve pouch‐type full batteries that deliver exceptional reversibility. The ARB process can, in principle, be applied to any metal chemistry to achieve similar crystallographic uniformity, provided the appropriate temperature and accumulated strains are employed. This concept is evaluated using commercial Li and Na foils, which, unlike Zn (HCP), are BCC crystals. The simple process for creating strong textures in both hexagonal and cubic metals and illustrating the critical role such built‐in crystallography plays underscores opportunities for developing highly reversible thin metal anodes (e.g., hexagonal Zn, Mg, and cubic Li, Na, Ca, Al).