Gemini surface active ionic liquids (GSAILs) are considered a new prosperous class of ionic liquids and recognized as high performance materials. The present study explores the capabilities of the newly synthesized GSAILs, constructed from two benzimidazole rings attached via a four or a six carbon spacer, namely [C4benzim-Cn-benzimC4][Br2], n = 4 and 6. The products were characterized with FT-IR, NMR, XRD, TGA, DTG and SEM methods and were used in curing interfacial properties of the crude oil– water system. The interfacial tension (IFT) was reduced to about 64 and 71% under critical micelle concentrations (CMCs) of 0.028 and 0.025 mol dm−3 at 298.2 K for n = 4 and 6 GSAILs, respectively. Temperature significantly assisted this effect. Both the GSAILs could transfer the wettability of the solid surface from oil-wet to water-wet. Further, stable oil/water emulsions were produced, having emulsion indices of 74.2 and 77.3% for n = 4 and 6 GSAILs, respectively. Compared to homologous imidazolium GSAILs, the benzimidazolium products revealed better performance in the sense of exhibiting desired effects on the investigated interfacial properties. These can be attributed to the stronger hydrophobicity of the benzimidazolium rings as well as better spreading of the molecular charges. The Frumkin isotherm could exactly reproduce the IFT data, leading to precise determination of the important adsorption and thermodynamic parameters.
