Oriented Zn plating guided by aligned ZnO hexagonal columns realizing dendrite-free Zn metal electrodes

Aqueous zinc-ion batteries (AZIBs), featuring low cost and high safety, have become a research hotspot in recent years. However, the low Zn stripping/plating reversibility, caused by dendritic growth, harmful side reactions, and Zn metal corrosion, severely influences the applicability of AZIBs. Zincophilic materials have shown great potential to form protective layers at the surface of Zn metal electrodes, whereas those protective layers are usually thick, lack fixed crystalline orientation, and require binders. Herein, a facile, scalable, and cost-effective solution method is used to grow vertically aligned ZnO hexagonal columns with (002) top surface and low thickness of 1.3 µm onto Zn foil. Such oriented protective layer can promote homogenous and nearly horizontal Zn plating not only on the top but also at the side of ZnO columns due to the low lattice mismatch between Zn (002) and ZnO (002) facets and between Zn (110) and ZnO (110) facets. Accordingly, the modified Zn electrode exhibits dendrite-free behavior with considerably suppressed corrosion issue, inert byproduct growth, and hydrogen evolution. Thanks to that, the Zn stripping/plating reversibility is significantly improved in Zn//Zn cell, Zn//Ti cell, and Zn//MnO2 battery. This work provides a promising avenue for guiding metal plating process via oriented protective layer.