Aligned Dipoles Induced Electric‐Field Promoting Zinc‐Ion De‐Solvation toward Highly Stable Dendrite‐Free Zinc‐Metal Batteries

Abstract Water‐induced parasitic reactions and uncontrolled dendritic Zn growth are long‐lasting tricky problems that severely hinder the development of aqueous zinc‐metal batteries. Those notorious issues are closely related to electrolyte configuration and zinc‐ion transport behavior. Herein, through constructing aligned dipoles induced electric‐field on Zn surface, both the solvation structure and transport behavior of zinc‐ions are fundamentally changed. The vertically ordered zinc‐ion migration trajectory and gradually concentrated zinc‐ion achieved inside the polarized electric‐field remarkably eliminate water related side‐reactions and Zn dendrites. Zn‐metal under the polarized electric‐field demonstrated significantly improve reversibility and a dendrite‐free surface with strong (002) Zn deposition texturing. Zn||Zn symmetric cell delivers greatly prolonged lifespan up to 1400 h (17 times longer than that of the cell based on bare Zn) while the Zn||Cu half‐cell demonstrate ultrahigh 99.9% coulombic efficiency. NH 4 V 4 O 10 ||Zn half‐cell delivered exceptional‐high 132 mAh g −1 capacity after ultralong 2000 cycles (≈100% capacity retention). In addition, MnO 2 ||Zn pouch‐cell under aligned dipoles induced electric‐field maintains 87.9% capacity retention after 150 cycles under practical condition of high MnO 2 mass loading (≈10 mg cm −2 ) and limited N/P ratio. It is considered that this new strategy can also be implemented to other metallic batteries and spur the development of batteries with long‐lifespan and high‐energy‐density.