Effective Orientation Control of the Zinc Anode for High-Performance Aqueous Zinc-Ion Batteries: A Key Approach To Address Dendrite Growth and Side Reactions

Aqueous zinc-ion batteries (AZIBs) are promising candidates for next-generation electrochemical energy storage systems owing to their abundant resources, high safety, great theoretical capacity, and environmental friendliness. Nonetheless, instability of Zn metal anodes caused by Zn dendrites and various side reactions poses a challenge to their practical feasibility. Optimizing the crystallographic orientation of the Zn metal anodes is demonstrated as a potential approach for solving these issues of AZIBs. Herein, we report an electrodeposition strategy to manipulate the exposure of the preferred (002) crystal planes in the artificial interface layer on Zn foil via adjustment of the electrodeposition current density and time. The (002)-oriented Zn metal anodes with an impressive 97.55% relative texture coefficient (RTC) value of (002) and ultrahigh I(002)/I(100) ratio of 310.23 were achieved through electrodeposition at a moderate current density of 30 mA cm–2 and electrodeposition time of 30 min, applicable to large-scale industrial production. The enhanced wettability of the designed (002) Zn@Zn anodes in electrolytes along with the low charge transfer resistance facilitates the migration of Zn2+ and guides the uniform Zn deposition, thereby inhibiting the dendrite growth and byproduct formation and promoting fast kinetics. In comparison to (101)-oriented pure Zn, the symmetric cell based on (002) Zn@Zn anodes exhibits ultrastable cycling for 3200 h at 1.0 mA cm–2, and the half-cell presents an average coulombic efficiency of 99.76% throughout the entire 3000 cycles at 5.0 mA cm–2. The full cell with a bismuth-doped manganese dioxide cathode exhibits an ultrastable cycling performance over 3500 cycles even at 10 C. This work proposes a strategy to regulate the preferred orientation of high-performance Zn anodes for advanced AZIBs.