Nature has demonstrated to be an extraordinary source of endless inspiration for designing and engineering a variety of complex and functional materials and systems to be used in numerous applications. Inspired by several fascinating and stimulating natural systems, which include the example of tobacco mosaic virus, or even the cell membrane, scientists have been boosted towards the development of increasingly complex supramolecular functional biomaterials aiming at addressing key biomedical and biotechnological applications, including tissue engineering, regenerative medicine, or drug delivery. In this work, we took advantage and maximize the use of materials from renewable sources, including polysaccharides, by developing novel hybrid supramolecular nanostructured multilayered biomaterials comprising high-molecular-weight biopolymers and oppositely charged low-molecular-weight self-assembling peptide amphiphile molecules, through combination of self-assembly and electrostatically-driven layer-by-layer (LbL) assembly approaches. Alginate, an anionic biocompatible polysaccharide extracted from brown seaweed, was used to trigger the self-assembling capability of positively charged peptide amphiphile molecule and formation of one-dimensional supramolecular nanofiber networks. Then, the LbL technology was employed to fabricate well-defined supramolecular multilayered biomaterials with tailored composition, thickness, and structure at the nanoscale by repeating the alternate deposition of both molecules. The buildup process was monitored <i>in situ</i> by quartz crystal microbalance with dissipation monitoring, which proved that both materials can be successfully combined to conceive stable supramolecular nanostructured multilayered systems. Their morphological properties were assessed by advanced microscopy techniques, revealing the nanostructured dimensions and one-dimensional nanofibrous network of the assembly formed by the two molecules. The <i>in vitro</i> biological performance of the supramolecular biomaterials was inspected using C2C12 myoblast cells. Enhanced cell adhesion, proliferation, and differentiation was observed on supramolecular systems having peptide amphiphile as the outermost layer. Our results suggest that such supramolecular biomaterials could be used in the near future as promising biomimetic supramolecular matrices for biomedical applications, including those in muscle tissue regeneration.

Bottom-up fabrication of hybrid polysaccharide/peptide amphiphile supramolecular multilayered biomaterials by combining self-assembly and layer-by-layer assembly approaches

253rd National Meeting (2017)

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