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The amphiphilic ionic liquids containing an alkyl chain in molecules form nano-structure in the bulk, although they also show surface activity and form aggregates in aqueous solutions. Although insights into the layer structures of ionic liquids were obtained using X-ray and neutron scattering techniques, the nanostructures of ionic liquids remain unclear. Herein, the surface adsorption and bulk properties of homogeneous polyoxyethylene (EO)-type nonionic surfactants (C  x  EO 6 ; x = 8, 12, or 16) were elucidated in quaternary-ammonium-salt-type amphiphilic gemini ionic liquids with oxygen or nitrogen-containing spacers [ 2 C  n  (Spacer) NTf 2 ; (Spacer) = (2-O-2), (2-O-2-O-2), (2-N-2), (2/2-N-2), (3), (5), or (6); n = 10, 12, or 14 for (2-O-2) and n = 12 for all other spacers] by surface tension, small- and wide-angle X-ray scattering, cryogenic transmission electron microscopy, and viscosity measurements. The surface tension of C 12 EO 6 in 2C  n  (Spacer) NTf 2 with oxygen-containing spacers increased with increasing concentration of C 12 EO 6 , becoming close to that of C 12 EO 6 alone, indicating that the amphiphilic ionic liquid adsorbed at the interface was replaced with C  x  EO 6 . In contrast, both 2C  n  (Spacer) NTf 2 with nitrogen-containing spacers and nonionic surfactants remained adsorbed at the interface at high concentrations. In the bulk, it was found that 2C  n  (Spacer) NTf 2 formed layer structures, in which the spacing depended on the alkyl chain length of C  x  EO 6 . These insights are expected to advance the practical applications of amphiphilic ionic liquids such as ion permeation, drug solubilization, and energy delivery systems.

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Surface Adsorption Properties and Layer Structures of Homogeneous Polyoxyethylene-Type Nonionic Surfactants in Quaternary-Ammonium-Salt-Type Amphiphilic Gemini Ionic Liquids with Oxygen- or Nitrogen-Containing Spacers