Controlling the molecular structure of biocompatible hydrogels by combining PAOxylation chemistry and Monte Carlo stochastic tools.

Hydrogels are three-dimensional networks of cross-linked hydrophilic copolymers. Their viscoelastic properties can be tailored by adjusting the chemical composition of the copolymers which build up the hydrogel. Poly(oxazoline)s (POx) are a class of low dispersity polymers. The poly(2-ethyl-2-oxazoline) is biocompatible, stealthy and non-toxic, which makes this hydrophilic polymer, as well as POx hydrogels interesting for various biomedical purposes. Experimental characterization tools only allow to determine average (co)polymer characteristics. Yet, it would be desirable to have a complete characterization of the (co)polymer microstructure for each macromolecule, at any time during the polymerization. This means that the composition of the copolymer backbone could be visualized, showing the location of all the reactive comonomers and/or branching points, and this for all individual branches/segments. A control of the microstructure during the synthesis of the copolymers allows for a relation of the microstructural parameters – (i) slope of transition (gradient or random copolymeric structure), (ii) pore size of hydrogels – to the performance of the final hydrogel material. In this way, the synthetic conditions can be optimized towards specific needs for the hydrogel material. This will be accomplished by implying a model-based design of POx hydrogels, using kinetic modeling through matrix-based computational techniques. This will produce state of the art POx hydrogel