Dendrites‐Free Zn Anode Enabled by Dense Zn Deposition and Spontaneous Texture Reconstruction on (110)‐Oriented Nanotwinned Cu

Abstract Uncontrollable zinc dendrite growth and limited utilization of the zinc metal anode have restricted the application of aqueous zinc‐ion batteries (AZIBs). Here, (110)‐oriented perpendicular aligned nanotwinned copper (P‐ntCu) current collector is fabricated by one‐step electrodeposition. High‐density twin boundaries (TBs) on the surface of P‐ntCu regulate dense zinc deposition by providing abundant nucleation sites and reducing the diffusion barrier for surface diffusion of zinc ions. The minimal lattice mismatch and interfacial energy between Zn(102) and Cu(110) facets results in a strong Zn(102) texture on P‐ntCu. This high‐density zinc undergoes spontaneous texture reconstruction from (102) to (002) during electrical cycling, which endows Zn@P‐ntCu with excellent dendrite‐free cycling and durability. As a result, the P‐ntCu current collector enables high stability with 99.91% coulombic efficiency and a long cycling stability of 2900 cycles at 5 mA cm −2 . The integrated Zn@P‐ntCu anode can be stably cycled for more than 3000 h (1 mA cm −2 , 1 mAh cm −2 ). This research provides a pathway for developing low‐cost and sustainable current collectors in AZIBs.