Aqueous rechargeable zinc (Zn) metal batteries show great application prospects in grid-scale energy storage devices due to their good safety, low cost, and considerable energy density. However, the electrical and topographical inhomogeneity caused by the native passivation layer of metallic Zn foil leads to inhomogeneous electrochemical plating and stripping of metallic Zn, and the limited accessible area to the electrolyte of the regular foil electrode causes the poor rate capability, which together hinder the practical application of the Zn metal electrode in rechargeable aqueous batteries. In this work, we show that the native passivation layer on the Zn foil electrode can be removed by a simple chemical polishing strategy, associated with the formation of a three-dimensional ridge-like structure of metallic Zn (r-Zn) on the surface of the Zn foil electrode due to the selective etching of weak crystallographic planes and grain boundary of metallic Zn. The clean and uniform surface of the metallic Zn electrode enables homogeneous plating and stripping of metallic Zn, and the ridge-like structure of r-Zn increases the accessible surface area to the electrolyte and reduces the local current density, which elevates the electrochemical performance of the Zn metal anode with regard to the cycling stability and rate capability. It is demonstrated that a r-Zn anode cycles stably for over 200 h at 1 mA cm-2 and 0.5 mA h cm-2 with a low overpotential of 20 mV, which far outperforms 39 h of cycling with an overpotential of 72 mV for its pristine metallic Zn counterpart.
Keywords: aqueous zinc metal battery; chemical polishing; homogeneous plating; passivation layer; ridge-like structure.