Biomimetic and multifunctional poly(glycerol sebacate)-based elastomeric hydrogels for soft tissue healthcare

A critical aspect in designing biomaterials with the advanced healthcare functionalities is their interaction with biology. In this regard, elastomers capable of responding to the various physiological dynamics in vivo are of significant interest in advanced soft tissue healthcare applications. In this thesis, new multifunctional biocompatible elastomers with bioactive and biomimetic behaviours were developed and characterised based on poly(glycerol sebacate) (PGS), for their potential soft tissue healthcare applications such as soft tissue engineering, wound healing, and drug delivery. The direct crosslinking and copolymerisation of the PGS pre-polymer and gelatin was studied by varying the ratio between PGS and gelatin. The biomimetic mechanical properties as well as an architecture of porous tissue scaffold illustrate their potential in soft tissue engineering. The pH-responsive water swelling property given by gelatin was further investigated in pH-responsive drug delivery applications. PGS-based polyurethane-clay nanocomposites with varying amounts of an organically modified clay were successfully synthesised on the modulation of physical properties of PGS. The synthesis was performed in a combined approach of the solvent method and in situ polymerisation. Hydration, mechanical, and degradable properties were improved with the addition of clay, illustrating its potential in soft tissue engineering. The selective drug loading and absorption behaviour was studied for controlled drug delivery application. Polyester-clay nanocomposites with different clay contents were developed. The hydration, hydrophilicity, and water vapour permeability were engineered with the addition of clay. Novel pro-angiogenic and malodourous diamine-controlling properties were also studied. Together with the porous foam structure, the potential of these new nanocomposites in the wound healing and soft tissue engineering applications was discussed. Overall, the new elastomers developed in this thesis based on PGS, exhibit great potentials in soft tissue healthcare applications with finely engineered or newly created properties on PGS.