Water-Controlled Structural Transition and Charge Transfer of Interfacial Ionic Liquids.

Clarification of the water-induced structural transitions and electron transfer between ionic liquids (ILs) and a solid surface allows for establishing a unified view of the electrical properties of interfacial ILs via a hitherto unexplored pathway. Here, we propose a simple and effective method to quantitatively identify and extract the transferred electrons between ILs and a solid surface, while demonstrating the critical structural transition of interfacial ILs from ordered stripe structures to disordered aggregation structures. The formation of hydrated anions, rooted in the hydrogen bonds of O-H···O between the anion and water, lies at the tipping point where electron transfer ends and aggregation structure begins.