Cartilage and Bone in Concert: Biofunctional Scaffolds for Osteochondral Regeneration

In this data repository, we have included the Supplementary Data of Chapters 3–7 of the associated dissertation (Cartilage and Bone in Concert: Biofunctional Scaffolds for Osteochondral Regeneration). The work described in this thesis focuses on the development of novel functional biomaterials in the context of osteochondral applications and additive manufacturing technologies. The first part of thesis is aimed at developing polymers with addressable groups on which ligands can be reacted post-processing. In Chapter 3, a two-step synthesis is reported of poly(ε-caprolactone)-azide (PCLA). In Chapter 4, PCL and PCL-maleimide scaffolds were produced with melt extrusion-based additive manufacturing. The surfaces were functionalized with ligands, and finally the effect of surface-grafted peptides on human mesenchymal stromal cell differentiation was investigated. Subsequently, in chapter 5, we explore a blending strategy to tune the surface-density of ligands on the surface of scaffolds. In the second part of the thesis, hydrogels comprising biologically relevant groups for articular cartilage applications were developed. We describe in chapter 6 the synthesis of sulfonated hyaluronic acid-based polymers and hydrogels. Finally, in chapter 7, the synthesis of novel copolymers is described with a tunable fraction of pendent sulfonate and aldehyde groups. In addition, we show the formation of strain-stiffening hydrogels using a hydrazide based crosslinker, ligand ligation, microfluidic printing, as well as the ability to replace hydrazone with oxime bonds via competitive binding.