Switching Hydrophobic Interface with Ionic Valves for Reversible Zinc Batteries

Abstract Developing hydrophobic interface has proven effective in addressing dendrite growth and side reactions during zinc (Zn) plating in aqueous Zn batteries. However, this solution inadvertently impedes the solvation of Zn²⁺ with H₂O and subsequent ionic transport during Zn stripping, leading to insufficient reversibility. Herein, an adaptive hydrophobic interface that can be switched “on” and “off” by ionic valves to accommodate the varying demands for interfacial H₂O during both the Zn plating and stripping processes, is proposed. This concept is validated using octyltrimethyl ammonium bromide (C₈TAB) as the ionic valve, which can initiatively establish and remove a hydrophobic interface in response to distinct electric‐field directions during Zn plating and stripping, respectively. Consequently, the Zn anode exhibits an extended cycling life of over 2500 h with a high Coulombic efficiency of ≈99.8%. The full cells also show impressive capacity retention of over 85% after 1 000 cycles at 5 A g⁻¹. These findings provide a new insight into interface design for aqueous metal batteries.