Abstract
Programmed to retain active responsivity to environmental stimuli,
diverse types of synthetic gels have been attracting interests regarding
various applications, such as versatile elastic biodevices. In a
different approach, when the gels are made of tissue-derived
biopolymers, they can act as an artificial extracellular matrix (ECM)
for use as soft implants in regenerative medicine. To explore the
physical properties of hydrogels in terms of statistical thermodynamics,
the mean-field Flory-Huggins-Rehner theory has long been used with
various analytical and numerical modifications. Here we suggest a novel
mathematical model on the volume phase transition of a biological hybrid
gel that is sensitive to ambient temperature. To mimic acellular soft
tissues, the ECM-like hydrogel is modeled as a network of biopolymer
chains, such as type I collagen and gelatin, which are covalently
crosslinked and swollen in aqueous solvents. Within the network,
thermoresponsive synthetic polymer chains are doped by chemical
conjugation. Based on the Flory-Huggins-Rehner framework, our model
phenomenologically illustrates a well-characterized volume phase
behavior of engineered tissue mimics as a function of temperature by
formulating the ternary mixing free energy of the polymer-solvent system
and by generalizing the elastic free energy term. With this formalism,
the decoupling of the Flory-Huggins interaction parameter between the
thermoresponsive polymer and ECM biopolymer enables deriving a simple
analytical equation for the volume phase transition as a function of the
structural and compositional parameters. We show that the doping ratio
of the thermoresponsive polymers affects the phase transition
temperature of the ECM-like gels.