We investigate the structure and interactions of a model
anionic/amphoteric
mixed surfactant micellar system, namely, sodium dodecyl sulfate (SDS)
and N,N-dimethyldodecylamine N-oxide (DDAO), employing SANS, FTIR, DLS, and pH measurements,
in the range 0.1–100 mM total surfactant concentration and
0–100% DDAO. Increasing surfactant concentration is found to
elongate the prolate ellipsoid micelles (R
Polar ∼ 25–40 Å), accompanied by up to a 6-fold increase
in micellar charge. The surfactant synergy, in terms of micellar charge
and size, diffusion coefficient, solution pH, and headgroup interactions,
was found to vary with concentration. At lower concentrations (≤50
mM), the SDS–DDAO ratio of maximum synergy is found to be asymmetric
(at 65–85% DDAO), which is rationalized using regular solution
theory, suggesting an equilibrium between Na+ dissociation,
DDAO protonation, and counterion concentration. At higher concentrations,
maximum synergy shifts toward the equimolar ratio. Overall, our study
expands and unifies previous reports, providing a comprehensive understanding
for this model, synergetic mixed micellar system.