Resilin is an elastic rubber‐like protein found in the cuticles of insects. It incorporates outstanding properties of high resilience and fatigue lifetime, where kinetic energy storage is needed for biological functions such as flight and jumps. Since resilin is rich in tyrosine groups, localized photopolymerization is enabled due to the ability to introduce di‐tyrosine bonds by a ruthenium‐based photoinitiator. Using Multiphoton Absorption Polymerization 3D printing process, objects containing 100% recombinant resilin protein are printed in water at a submicron length scale. Consequently, protein‐based hydrogels with complex structures are printed using space positioning voxel polymerization. The objects are characterized by dynamic mechanical analysis using nanoindentation. Printing parameters such as printing speed and laser power are found to enable tuning the mechanical properties of the printed objects. The printed objects are soft and resilient, similar to native resilin, while presenting the highest resolution of a structure made entirely of a protein and better mechanical properties of common hydrogels and poly(dimethylsiloxane). Moreover, topography and mechanical properties enable cell growth and alignment without cell adhesion primers, thus facilitating biological applications. The fabrication of 3D resilin‐based hydrogel will open the way for potential applications based on biomimicking and in creating new functional objects.
Hydrogels have been proposed as potential candidates for many different applications. However, many hydrogels exhibit poor mechanical properties, which limit their applications. Recently, various cellulose-derived nanomaterials have emerged as attractive candidates for nanocomposite-reinforcing agents due to their biocompatibility, abundance, and ease of chemical modification. Due to abundant hydroxyl groups throughout the cellulose chain, the grafting of acryl monomers onto the cellulose backbone by employing oxidizers such as cerium(IV) ammonium nitrate ([NH4]2[Ce(NO3)6], CAN) has proven a versatile and effective method. Moreover, acrylic monomers such as acrylamide (AM) may also polymerize by radical methods. In this work, cerium-initiated graft polymerization was applied to cellulose-derived nanomaterials, namely cellulose nanocrystals (CNC) and cellulose nanofibrils (CNF), in a polyacrylamide (PAAM) matrix to fabricate hydrogels that display high resilience (~92%), high tensile strength (~0.5 MPa), and toughness (~1.9 MJ/m3). We propose that by introducing mixtures of differing ratios of CNC and CNF, the composite’s physical behavior can be fine-tuned across a wide range of mechanical and rheological properties. Moreover, the samples proved to be biocompatible when seeded with green fluorescent protein (GFP)-transfected mouse fibroblasts (3T3s), showing a significant increase in cell viability and proliferation compared to samples comprised of acrylamide alone.
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