Microstructure of supercritical CO2-in-water microemulsions: a systematic contrast variation study

Abstract

Microemulsions of the type H₂O–scCO₂–surfactant are potential candidates for novel solvent mixtures in the field of green chemistry. Furthermore, scCO₂-microemulsions are highly interesting from a fundamental point of view since their properties such as the bending elastic constants can be strongly influenced solely by varying the pressure without changing the components. With this motivation we studied the phase behavior and the microstructure of water-rich scCO₂-microemulsions. Such microemulsions were formulated using the technical grade non-ionic surfactants Zonyl FSO 100 and Zonyl FSN 100. At elevated pressures the temperature dependent phase behavior of these systems follows the general patterns of non-ionic microemulsions. Small angle neutron scattering experiments were conducted to determine the length scales and the topology of the microstructure of these systems. Having determined the exact scattering length densities and the composition of the respective sub-phases by a systematic contrast variation we could show that these systems consist of CO₂-swollen microemulsion droplets that are dispersed in a continuous aqueous-phase. The scattering data were analyzed using a newly derived form factor for polydisperse, spherical core/shell particles with diffuse interfaces. The underlying analytical density profiles could be confirmed applying the model-free Generalized Indirect Fourier Transformation (GIFT) to the scattering data. Following the general patterns of non-ionic microemulsions the radius of the microemulsion droplets is found to increase almost linearly upon the addition of CO₂.