Vertical Crystal Plane Matching between AgZn3 (002) and Zn (002) Achieving a Dendrite‐Free Zinc Anode

Abstract Metallic zinc anodes in zinc‐ion batteries suffer from problematic Zn dendrite chemistry. Previous works have shown that preferred‐orientation crystal planes can help dendrite‐free metal anodes. This work reports a nanothickness (≈570 nm) AgZn 3 coating to regulate the Zn growth. First, AgZn 3 @Zn anode avoids the problem, in Ag@Zn anode, that the rate of electrochemical Ag‐Zn alloying is slower than that of Zn dendrites growth. Batteries life increased from 112 h (pure Zn) and 932 h (Ag@Zn) to 1360 h (AgZn 3 @Zn) at 2 mA cm −2 and 1 mAh cm −2 . Then, plasma sputtering can remove nonconductive ZnO and improve Zn‐ion affinity, which brings a longer life for AuZn 3 @Zn (423 h), CuZn 3 @Zn (385 h), and AgZn 3 @Zn (1150 h) than pure Zn (93 h) at 1 mAh cm −2 . More importantly, AgZn 3 (002) has a high matching with the Zn (002), which can guide ordered Zn epitaxial deposition, thereby achieving dense and dendrite‐free Zn growth. This work clearly captures the fascinating structure of the densely stacked Zn layers on the AgZn 3 layer. This strategy not only improves the performance of zinc‐ion batteries greatly but will also help one understand the matching mechanism of the (002) vertical crystal plane.