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 center dot center dot center dot O between the anion and water, lies at the tipping point where electron transfer ends and aggregation structure begins. In addition, it is discovered to what extent the hydrophilicity of substrates can affect electron transfer, and a regulation method based on the electric field is explored. These experimental findings may refresh our knowledge of interfacial ILs and provide an effective method for evaluating the intrinsic electrical features of the ILs-solid surface.

Automated summary

This study clarifies the structural transitions and electron transfer between ionic liquids (ILs) and a solid surface, providing a unified understanding of the electrical properties of interfacial ILs. It is found that the formation of hydrated anions marks the tipping point between electron transfer and aggregation structure, while the hydrophilicity of substrates affects the extent of electron transfer. Additionally, a regulation method based on the electric field is proposed.