About entangled networks of worm like micelles: A rejected hypothesis

We report new results from small-angle neutron scattering on d(1 2)-cyclohexane/lecithin/water micellar solutions performed as a function of the water content (w(o)), temperature (T) and dispersed phase volume fraction (phi). The data from dilute samples are interpretable in terms of the existence of giant cylindrical reverse micelles and are well fit with a core-shell model (that provides the micelle structure and dimensions) with values of 28 and 45 Angstrom for the inner core and the outer shell radii, almost independent on temperature and concentration. Such a result could appear consistent with the current idea that worm-like micelles are living polymers. On the contrary, the appearance of a sharp interference maximum at high concentrations (phi > 0.15) suggests arguments against the current hypothesis of an entangled network of giant flexible cylinders. Further arguments against the current hypothesis are given by the close similarity between the above described results and those from free of water micelles (for sure not cylinders). All the data are well fitted in terms of a unique model taking into account the micellar form factor plus a hard sphere structure factor. The data analysis suggests a micellar size distribution determined by the competition between concentration and interaction effects on which temperature plays not a minor role. Following our results, the current hypothesis of a gel structure in terms of an entangled network can be assumed as wrong and some caution has to be taken in assuming wormlike micelles as living polymers.