Interfacial Forces across Ionic Liquid Solutions: Effects of Ion Concentration and Water Domains †

Using the surface force apparatus (SFA), the interaction forces between mica surfaces across ionic liquid (IL) solutions are studied. The IL solution, 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide in propylene carbonate solvent, is used at different concentrations to elucidate the ions' conformation at the interface from the analysis of short-range structural forces. A direct correlation between the ion layer thickness at the interface and the IL molar fraction in the solution is observed, suggesting conformational changes relative to the ion packing density. In addition, effects of large microscopic and macroscopic water domains at the interface are investigated. The microscopic water domains induced significant adhesion at contact because of the long-range capillary forces, which are found to depend on solvent concentration. The macroscopic water domains entirely cover the interaction area, ensuring that the long-range interfacial interactions occur entirely across the aqueous electrolyte solution with dissolved IL ions as the electrolyte. These results help elucidate the interfacial interactions in IL-charged solid interfaces with practical importance in green energy storage, catalysis, and lubrication.