Unveiling Contact‐Electrification Effect on Interfacial Water Oscillation

Abstract Water is crucial for various physicochemical processes at the liquid–solid interfaces. In particular, the interfacial water, mediating the electric field and solvation effect along with the solid, corporately determine the electrochemical properties. Understanding the interaction between solid properties and the interface water holds significant importance in interfacial dynamics. However, the impact of alterations in the charged state of solid surfaces induced by contact electrification on interfacial water remains unknown. Here, the evolution of atomic‐level resolution maps of hydration layers are reported on charged surfaces using 3D atomic force microscopy (3D‐AFM). These findings demonstrate that electrostatic interactions can reinforce, distort, or collapse the characteristic structure of hydration layers. More importantly, these interactions exhibit interlayer differences and sample specificity in hydration layer structures of different substrates. In addition, similar oscillations of the hydration layer are observed at the electrochemical interface under different voltage biases. This suggests that contact‐electrification has the potential to serve as a novel method for manipulating and regulating chemical reactions at the interface.