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Polyelectrolyte-surfactant mixtures and their interactions with fluid interfaces are an important research field due to their use in technological applications. Most of the existing knowledge on these systems is based on models in which the polyelectrolyte concentration is around 50 times lower than that used in commercial formulations. The present work marks a step to close the gap on the understanding of their behavior under more practically-relevant conditions. The adsorption of concentrated mixtures of poly(diallyldimethyl-ammonium) chloride and sodium N-lauroyl-N-methyltaurate at the water/vapor interface with a crude mixing protocol has been studied by different surface tension techniques, Brewster angle microscopy, neutron reflectometry, and several bulk characterization techniques. Kinetically-trapped aggregates formed during mixing influence the interfacial morphology of mixtures produced in the equilibrium one-phase region, yet fluctuations in the surface tension isotherm result depending on the tensiometric technique applied. At low bulk surfactant concentrations, the free surfactant concentration is very low, and the interfacial composition matches the trend of the bulk complexes, which is a behavior that has not been observed in studies on more dilute mixtures. Nevertheless, a transition to synergistic co-adsorption of complexes and free surfactant is observed at the higher bulk surfactant concentrations studied. This transition appears to be a special feature of these more concentrated mixtures, which deserves attention in future studies of systems with additional components.

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We report here a review of particle-laden interfaces. We discuss the importance of the particle’s wettability, accounted for by the definition of a contact angle, on the attachment of particles to the fluid interface and how the contact angle is strongly affected by several physicochemical parameters. The different mechanisms of interfacial assembly are also addressed, being the adsorption and spreading the most widely used processes leading to the well-known adsorbed and spread layers, respectively. The different steps involved in the adsorption of the particles and the particle-surfactant mixtures from bulk to the interface are also discussed. We also include here the different equations of state provided so far to explain the interfacial behavior of the nanoparticles. Finally, we discuss the mechanical properties of the interfacial particle layers via dilatational and shear rheology. We emphasize along that section the importance of the shear rheology to know the intrinsic morphology of such particulate system and to understand how the flow-field-dependent evolution of the interfacial morphology might eventually affect some properties of materials such as foams and emulsions. We dedicated the last section to explaining the importance of the particulate interfacial systems in the stabilization of foams and emulsions.

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