Clickable Dynamic Bioinks Enable Post‐Printing Modifications of Construct Composition and Mechanical Properties Controlled over Time and Space

Bioprinting is an emerging technology that holds promise for applications in both tissue engineering and regenerative medicine. One of the main challenges in bioprinting research is reliance on non-physiological stimuli or sacrificial baths, as well as difficulties associated with adjusting the composition and mechanical properties of the biomaterials available for printing. This paper presents a new type of biomaterial called “clickable dynamic bioinks” to overcome current challenges in the field. These bioinks are based on dynamic hydrogels, allowing for both printability and subsequent chemical modification through click reactions after printing, thereby enabling targeted changes to the physical and biochemical properties of the printed constructs. Using hyaluronic acid (HA) as the

primary polymer, this work explores a boronate ester crosslinking mechanism to produce cytocompatible and printably dynamic hydrogels. The resultant dynamic bioinks are designed with bioorthogonal click groups to permit a wide range of post-printing modifications with corresponding click-functionalized molecules. Demonstrations of proof of concept include post-printing modification of polymer composition (e.g. HA, chondroitin sulfate, gelatin), stiffness modulation, and cell adhesion enhancement via peptide immobilization. These results illustrate the potential of dynamic bioinks for spatiotemporal control of the properties of printed constructs.

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