Nanoparticle/Polyelectrolyte Complexes for Biomimetic Constructs

Constructing all-aqueous systems with tailored geometries can generate a new class of biomimetic materials, a fascinating but challenging goal to achieve. Here, by taking advantage of the interfacial complexation of a polyelectrolyte (PE) and cellulose nanocrystals (CNCs), a unique interfacial PE/CNC complex is demonstrated for the stabilization of aqueous two-phase systems and for the fabrication of all-aqueous double emulsions and 3D constructs. The thickness of PE/CNC complex can be effectively adjusted by tuning the osmotic stress imbalance between the two aqueous phases and, during the formation and thickening of PE/CNC complex, individual assemblies can be connected to design hierarchical all-aqueous structures. This new platform affords tremendous potential for engineering biomimetic constructs with advanced functionality, that can be used for chemical separation, delivery, and biphasic cascading reaction vessels.