Microgel particles stabilised high internal phase emulsions for applications in tissue engineering
File(s)
Author(s)
Yuan, Wei
Type
Thesis or dissertation
Abstract
Tissue engineering using polymeric scaffolds to support cell growth and tissue regeneration is currently under development as a promising solution to tissue loss or organ failure. This thesis focuses on fabricating multifunctional scaffolds for tissue engineering using emulsion templating.
Poly(N-isopropylacrylamide-co-acrylic acid) [poly(NIPAAm-co-AA)] microgel particles were found capable of stabilising both w/o and o/w high internal phase emulsions (HIPEs), depending on the temperature, pH and salt concentration. PolyHIPEs were prepared by photo-polymerisation of both HIPEs containing monomers in the continuous phase and exhibited pore structures with sizes of a few hundred micrometers. For oil-soluble monomers, e.g., divinylbenzene (DVB), microgel particles stabilised w/o HIPEs were obtained at 40 °C using a microgel suspension (0.4 wt %) in 1 mM KCl solution at pH 4. For water-soluble monomers, e.g., potassium acrylate (KAA), the crosslinker content was found crucial to the formation of an open porous structure in poly(KAA) HIPEs. It was shown by cryo-scanning electron microscopy that the interconnections were not generated upon polymerisation but during solvent extraction. Highly interconnected poly(KAA) HIPEs prepared using 80 vol % internal phase possessed a low density of ca. 0.03 g/cm3 and a porosity up to 97~98%.
By using active ingredient (A.I.) loaded microgel particles as emulsifiers, polyHIPEs with delivery functionality were developed. The emulsifying ability of A.I. loaded microgels was found to be dependent on A.I.-microgel interactions. Paracetamol drug loaded microgel particles resulted in stable o/w HIPEs at either low (400 rpm) or high stirring speed (1000 rpm) and hence polyHIPEs with tunable morphologies after polymerisation.
Microgel particles stabilised o/w HIPEs were also used to fabricate macroporous dextran and dextran-co-polyNIPAAm. The pH of the aqueous phase was found crucial to HIPE stability and pH 6.8 resulted in stable HIPEs without coalescence and macropores with narrow pore size distribution after freeze-drying. By thermostating HIPEs prior to freezing or by varying dextran concentration, the morphology of macroporous dextran was tunable. Macroporous dextran-co-polyNIPAAm could potentially be used as a multiply responsive scaffold. Besides the stimuli-responsiveness of microgel particles, polyNIPAAm segments of the copolymers enabled scaffold integrity in water at physiological temperature.
Microgel particles stabilised HIPEs were established as a truly versatile template to fabricate macroporous polymers for potential applications as tissue engineering scaffolds.
Poly(N-isopropylacrylamide-co-acrylic acid) [poly(NIPAAm-co-AA)] microgel particles were found capable of stabilising both w/o and o/w high internal phase emulsions (HIPEs), depending on the temperature, pH and salt concentration. PolyHIPEs were prepared by photo-polymerisation of both HIPEs containing monomers in the continuous phase and exhibited pore structures with sizes of a few hundred micrometers. For oil-soluble monomers, e.g., divinylbenzene (DVB), microgel particles stabilised w/o HIPEs were obtained at 40 °C using a microgel suspension (0.4 wt %) in 1 mM KCl solution at pH 4. For water-soluble monomers, e.g., potassium acrylate (KAA), the crosslinker content was found crucial to the formation of an open porous structure in poly(KAA) HIPEs. It was shown by cryo-scanning electron microscopy that the interconnections were not generated upon polymerisation but during solvent extraction. Highly interconnected poly(KAA) HIPEs prepared using 80 vol % internal phase possessed a low density of ca. 0.03 g/cm3 and a porosity up to 97~98%.
By using active ingredient (A.I.) loaded microgel particles as emulsifiers, polyHIPEs with delivery functionality were developed. The emulsifying ability of A.I. loaded microgels was found to be dependent on A.I.-microgel interactions. Paracetamol drug loaded microgel particles resulted in stable o/w HIPEs at either low (400 rpm) or high stirring speed (1000 rpm) and hence polyHIPEs with tunable morphologies after polymerisation.
Microgel particles stabilised o/w HIPEs were also used to fabricate macroporous dextran and dextran-co-polyNIPAAm. The pH of the aqueous phase was found crucial to HIPE stability and pH 6.8 resulted in stable HIPEs without coalescence and macropores with narrow pore size distribution after freeze-drying. By thermostating HIPEs prior to freezing or by varying dextran concentration, the morphology of macroporous dextran was tunable. Macroporous dextran-co-polyNIPAAm could potentially be used as a multiply responsive scaffold. Besides the stimuli-responsiveness of microgel particles, polyNIPAAm segments of the copolymers enabled scaffold integrity in water at physiological temperature.
Microgel particles stabilised HIPEs were established as a truly versatile template to fabricate macroporous polymers for potential applications as tissue engineering scaffolds.
Version
Imperial Users Only
Date Issued
2010-11
Date Awarded
2015-02
Advisor
Steinke, Joachim
Sponsor
Engineering and Physical Sciences Research Council
Grant Number
EP/E007538/1
Publisher Department
Chemistry
Publisher Institution
Imperial College London
Qualification Level
Doctoral
Qualification Name
Doctor of Philosophy (PhD)