Natural Polysaccharides as Multifunctional Components for One-Step 3D Printing Tough Hydrogels

Natural polysaccharides (NPS) are regarded as biomolecular and structural components for preparing high-performance tough hydrogels. But the one-step fabrication of NPS-containing hydrogels in seconds and the template-free design of complicated high-resolution structures are still significant challenges in this field. To meet these requirements, various NPS-containing tough hydrogels are fabricated and processed into 2D/3D structures via the combination of Ru(bpy)₃²⁺-mediated photochemistry and extrusion 3D printing technique. The whole fabrication process is one-step, completed in tens of seconds under visible light irradiation. It is found that the used NPS plays a key role in achieving the fabrication of high-performance structured tough hydrogels. The high reactivity of functional groups in the used NPS can shorten their gelation times. Long rigid chains of the used NPS, their hierarchical assemblies, and contrasting multinetworks benefit from the efficient dissipation of mechanical energy and enhancement of its operational stability. Strong supramolecular interactions enable hydrogel precursors to have high viscosities, therefore providing good controllability to design high-resolution and complicated tough hydrogel structures via extrusion 3D printing. It is anticipated that this straightforward fabrication strategy and findings will open new horizons for NPS-containing materials.