3D printing of glycerol-mediated alginate hydrogels with high strength and stiffness

As a biomass material with biodegradability and biocompatibility, sodium alginate (SA) is a good candidate for constructing hydrogels for tissue-mimicking and biomedical scaffold fabricating through extrusion-based 3D printing technology. However, the mechanical strength and stiffness of alginate hydrogels are still not comparable with biological tissues such as tendons and the printability of SA solutions is often poor. Here, a novel strategy for 3D printing of alginate hydrogels with high mechanical performance is developed by using glycerol as a co-solvent for SA solutions. The addition of glycerol (GL) enables the formation of a homogenous SA/GL solution with a high solid content of 12-20 wt.% and endows crosslinked SA hydrogels with high stretchability. By applying uniaxial stretches, hydrogel filaments prepared with concentrated SA/GL solutions reveal a high tensile strength of 36.6-161.3 MPa, Young's modulus of 59.2-1964.2 MPa, and elongation at break of 8.5%-106.2% due to the high orientated and closely packed SA chains. SA/GL solutions become more solid-like with increasing SA concentration, and the solution with a solid content of 16 wt.% exhibits optimal 3D printability because of the appropriate rheological properties and thixotropic behavior. By designing the deforming-and-fixing process, 3D printed high-strength alginate hydrogels with complex structures are prepared, broadening the application of alginate hydrogels in load-bearing and biomedical fields.