Polydopamine Inter-Fiber Networks: New Strategy for Producing Rigid, Sticky, 3D Fluffy Electrospun Fibrous Polycaprolactone Sponges

Designing versatile 3D interfaces that can precisely represent a biological environment is a prerequisite for the creation of artificial tissue structures. To this end, electrospun fibrous sponges, precisely mimicking an extracellular matrix and providing highly porous interfaces, have capabilities that can function as versatile physical cues to regenerate various tissues. However, their intrinsic features, such as sheet-like, thin, and weak structures, limit the design of a number of uses in tissue engineering applications. Herein, a highly facile methodology capable of fabricating rigid, sticky, spatially expanded fluffy electrospun fibrous sponges is proposed. A bio-inspired adhesive material, poly(dopamine) (pDA), is employed as a key mediator to provide rigidity and stickiness to the 3D poly(e-caprolactone) (PCL) fibrous sponges, which are fabricated using a coaxial electrospinning with polystyrene followed by a selective leaching process. The iron ion induced oxidation of dopamine into pDA networks interwoven with PCL fibers results in significant increases in the rigidity of 3D fibrous sponges. Furthermore, the exposure of catecholamine groups on the fiber surfaces promotes the stable attachment of the sponges on wet organ surfaces and triggers the robust immobilization of biomolecules (e.g., proteins and gene vectors), demonstrating their potential for 3D scaffolds as well as drug delivery vehicles. Because fibrous structures are ubiquitous in the human body, these rigid, sticky, 3D fibrous sponges are good candidates for powerful biomaterial systems that functionally mimic a variety of tissue structures.