3D-Printed Hydrogels with High-Strength and Anisotropy Mediated by Chain Rigidity

Extrusion-based 3D printing is a facile technology to construct complex structures of hydrogels, especially for tough hydrogels that have shown demonstrated potential in load-bearing materials and tissue engineering. However, 3D-printed hydrogels often possess mechanical properties that do not guarantee their usage in tissue-mimicking, load-bearing components, and motion sensors. This study proposes a novel strategy to construct high-strength and anisotropic Fe 3+ cross-linked poly(acrylamide- co -acrylic acid)/sodium alginate double network hydrogels. The semi-flexible sodium alginate chains act as a “conformation regulator” to promote the formation of strong intermolecular interactions between polymer chains and lock the more extended conformation exerted by the pre-stretch, enabling the construction of 3D-printed hydrogel structures with high orientation. The equilibrated anisotropic hydrogel filaments with a water content of 50–60 wt.% exhibit outstanding mechanical properties (tensile strength: 9–44 MPa; elongation at break: 120–668%; Young's modulus: 7–62 MPa; toughness: 26–52 MJ m − 3 ). 3D-printed anisotropic hydrogel structures with high mechanical performance show demonstrated potential as loading-bearing structures and electrodes of flexible triboelectric nanogenerators for versatile human motion sensing.