Printable homocomposite hydrogels with synergistically reinforced molecular-colloidal networks

Austin H. Williams, Sangchul Roh, Alan R. Jacob, Simeon D. Stoyanov, Lilian Hsiao and Orlin D. Velev ()
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Austin H. Williams: North Carolina State University
Sangchul Roh: North Carolina State University
Alan R. Jacob: North Carolina State University
Simeon D. Stoyanov: North Carolina State University
Lilian Hsiao: North Carolina State University
Orlin D. Velev: North Carolina State University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract The design of hydrogels where multiple interpenetrating networks enable enhanced mechanical properties can broaden their field of application in biomedical materials, 3D printing, and soft robotics. We report a class of self-reinforced homocomposite hydrogels (HHGs) comprised of interpenetrating networks of multiscale hierarchy. A molecular alginate gel is reinforced by a colloidal network of hierarchically branched alginate soft dendritic colloids (SDCs). The reinforcement of the molecular gel with the nanofibrillar SDC network of the same biopolymer results in a remarkable increase of the HHG’s mechanical properties. The viscoelastic HHGs show >3× larger storage modulus and >4× larger Young’s modulus than either constitutive network at the same concentration. Such synergistically enforced colloidal-molecular HHGs open up numerous opportunities for formulation of biocompatible gels with robust structure-property relationships. Balance of the ratio of their precursors facilitates precise control of the yield stress and rate of self-reinforcement, enabling efficient extrusion 3D printing of HHGs.

Date: 2021
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DOI: 10.1038/s41467-021-23098-9

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