Stable Zn Anodes with Triple Gradients

Abstract Aqueous zinc‐ion batteries are highly desirable for sustainable energy storage, but the undesired Zn dendrites growth severely shortens the cycle life. Herein, a triple‐gradient electrode that simultaneously integrates gradient conductivity, zincophilicity, and porosity is facilely constructed for a dendrite‐free Zn anode. The simple mechanical rolling‐induced triple‐gradient design effectively optimizes the electric field distribution, Zn 2+ ion flux, and Zn deposition paths in the Zn anode, thus synergistically achieving a bottom‐up deposition behavior for Zn metals and preventing the short circuit from top dendrite growth. As a result, the electrode with triple gradients delivers a low overpotential of 35 mV and operates steadily over 400 h at 5 mA cm ‐2 /2.5 mAh cm ‐2 and 250 h at 10 mA cm ‐2 /1 mAh cm ‐2 , far surpassing the non‐gradient, single‐gradient and dual‐gradient counterparts. The well‐tunable materials and structures with the facile fabrication method of the triple‐gradient strategy will bring inspiration for high‐performance energy storage devices.