Synthesis and Processing of Dynamic Covalently Crosslinked Polydextran/Carbon Dot Nanocomposite Hydrogels with Tailorable Microstructures and Properties

Using functionalized nanoparticles to crosslink hydrophilic polymers is a growing theme of directly constructing nanocomposite (NC) hydrogels. Employing dynamic covalent chemistry at the nanoparticle-polymer interface is particularly attractive due to the spontaneous formation and reversible manner of dynamic covalent bonds. However, the structure and property modulation of the dynamic covalently crosslinked NC hydrogels has not been thoroughly discussed. Here, we fabricated NC hydrogels by using amine-functionalized carbon dots (CDs) to crosslink polydextran aldehyde (PDA) polymers through imine bond formation. The role of PDA with different oxidation degrees (i.e., PDA10, PDA30, and PDA50) in affecting the microstructures and properties of PDA@CD hydrogels was systematically investigated, showing that the PDA50@CD hydrogel presented the densest structure and the highest mechanical strength among the three PDA@CD hydrogels. The pH-responsiveness, 3D printing, electrospinning, and biocompatibility of PDA@CD hydrogels were also demonstrated, showing the great promise of using PDA@CD hydrogels for applications in biomedicine and biofabrication.