Utilizing the Natural Composition of Brown Seaweed for the Preparation of Hybrid Ink for 3D Printing of Hydrogels

This study aims to utilize the natural composition of brown seaweed by deriving alginate and cellulose concurrently from the stipe (stem-like) and blade (leaf-like) structures of the seaweed; further, this is followed by fibrillation for the direct and resource-efficient preparation of alginate/cellulose nanofiber (CNF) hybrid inks for three-dimensional (3D) printing of hydrogels. The efficiency of the fibrillation process was evaluated, and the obtained gels were further studied with regard to their rheological behavior. As a proof of concept, the inks were 3D printed into discs, followed by cross-linking with CaCl₂ to form biomimetic hydrogels. It was shown that the nanofibrillation process from both seaweed structures is very energy-efficient, with an energy demand lower than 1.5 kW h/kg, and with CNF dimensions below 15 nm. The inks displayed excellent shear-thinning behavior and cytocompatibility and were successfully printed into 3D discs that, after cross-linking, exhibited an interconnected network structure with favorable mechanical properties, and a cell viability of 71%. The designed 3D biomimetic hydrogels offers an environmentally benign, cost-efficient, and biocompatible material platform with a favorable structure for the development of biomedical devices, such as 3D bio printing of soft tissues.