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Chemical surfactants are omnipresent in consumers' products but they sufferfrom environmental concerns. For this reason, complete replacement ofpetrochemical surfactants by biosurfactants constitute a holy grail but this isfar from occurring any soon. If the "biosurfactants revolution" has notoccurred, yet, mainly due to the higher cost and lower availability ofbiosurfactants, another reason explains this fact: the poor knowledge of theirproperties in solution. This tutorial review aims at reviewing theself-assembly properties and phase behavior, experimental (sections 2.3 and2.4) and from molecular modelling (section 5), in water of the most importantmicrobial biosurfactants (sophorolipids, rhamnolipids, surfacting,cellobioselipids, glucolipids) as well as their major derivatives. A criticaldiscussion of such properties in light of the well-known packing parameter ofsurfactants is also provided (section 2.5). The relationship between thenanoscale self-assembly and macroscopic materials properties, includinghydrogelling, solid foaming, templating or encapsulation is specificallydiscussed (section 2.7). We also present their self-assembly and adsorption atflat and complex air/liquid (e.g., foams), air/solid (adhesion), liquid/solid(nanoparticles) and liquid/liquid (e.g., emulsions) interfaces (section 3). Acritical discussion on the use of biosurfactants as capping agents for thedevelopment of stable nanoparticles is specifically provided (section 3.2.4).Finally, we discuss the major findings involving biosurfactants andmacromolecules, including proteins, enzymes, polymers and polyelectrolytes.

Self-Assembly, Interfacial Properties, Interactions with Macromolecules  and Molecular Modelling and Simulation of Microbial Bio-based Amphiphiles  (Biosurfactants). A Tutorial Review