Inducing the Preferential Growth of Zn (002) Plane for Long Cycle Aqueous Zn‐Ion Batteries

Abstract Uncontrolled growth of Zn dendrites is the main reason for the short‐circuit failure of aqueous Zn‐ion batteries. Using electrolyte additives to manipulate the crystal growth is one of the most convenient strategies to mitigate the dendrite issue. However, most additives would be unstable during cycling due to the structural reconstruction of the deposition layer. Herein, it is proposed to use 1‐butyl‐3‐methylimidazolium cation (BMIm + ion) as an electrolyte additive, which could steadily induce the preferential growth of (002) plane and inhibit the formation of Zn dendrites. Specifically, BMIm + ion will be preferentially adsorbed on (100) and (101) planes of Zn anodes, forcing Zn 2+ ion to deposit on the (002) plane, thus inducing the preferential growth of the (002) plane and forming a flat and compact deposition layer. As a result, the Zn anode cycles for 1000 h at10 mA cm −2 and 10 mAh cm −2 as well as a high Coulombic efficiency of 99.8%. Meanwhile, the NH 4 V 4 O 10 ||Zn pouch cell can operate stably for 240 cycles at 0.4 A g −1 . The BMIm + ion additive keeps a stable effect on the structural reconstruction of the Zn anode during the prolonged cycling.