Interplay of Hydrogen Bonding and Hydrophobic Interactions to Control the Mechanical Properties of Polymer Multilayers at the Oil–Water Interface

We probe the mechanical shear and compression properties of hydrogen-bonded polymer multilayers directly assembled at the oil–water interface using interfacial rheology techniques. We show that the polymer multilayers behave mechanically like a transient network, with elastic moduli that can be varied over 2 orders of magnitude by controlling the type and strength of physical interactions involved in the multilayers, which are controlled by the pH and the hydrophobicity of the polymer. Indeed, the interplay of hydrogen and hydrophobic interactions enables one to obtain a tighter and stronger network at the interface. Moreover, we show how a simple LBL process applied directly on emulsion droplets leads to encapsulation of a model oil, dodecane, as well as perfume molecules.