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The aggregation behavior was investigated in mixtures of sodium dodecyl sulfate (SDS) and cetyltrimethylammonium bromide (CTAB) (anionic-rich catanionic) solutions. The study was conducted in solutions of water–ethylene glycol (EG) by means of surface tension, conductometry, cyclic voltammetry, zeta potential measurements, transmission electron microscopy (TEM) and dynamic light scattering (DLS) techniques. The degree of counterion dissociation ( α ), critical micelle concentration, aggregation numbers, interfacial properties, interparticle interaction parameters, and morphology of aggregates were determined. Based on regular solution theory, the cosolvent effects between SDS and CTAB as surfactants were also analyzed for both mixed monolayers at mixed micelles ( β  M ) and the air/liquid interface ( β  σ ). It was shown that the formation of large aggregates occurred in the presence of an excess of anionic surfactant. A phase transition from cylindrical micelles to spherical micelles in the anionic-rich regime was observed with an increase in the EG volume fraction. The inter particle interactions were assessed in terms of cosolvent effects on the micellar surface charge density and the cylindrical-to-spherical morphology change. Zeta potential and size of the aggregates were determined using dynamic light scattering and confirmed the models suggested for the processes taking place in each system.

Co-solvent Effect on Spontaneous Formation of Large Nanoscale Structures in Catanionic Mixtures in the Anionic-Rich Region