Abstract
This study reports the first fully synthetic fluid gel (SyMGels) using a simple poly(ethylene glycol) polymer. Fluid gels are an interesting class of materials: structured during gelation via shear-confinement to form microparticulate suspensions, through a bottom-up approach. Structuring in this way, when compared to first forming a gel and subsequently breaking it down, results in the formation of a particulate dispersion with particles "grown" in the shear flow. Resultantly, systems form a complex microstructure, where gelled particles concentrate remaining non-gelled polymer within the continuous phase, creating an amorphous-like interstitial phase. As such, these materials demonstrate mechanical characteristics typical of colloidal glasses, presenting solid-like behaviors at rest with defined yielding; likely through intrinsic particle-particle and particle-polymer interactions. To date, fluid gels have been fabricated using polysaccharides with relatively complex chemistries, making further modifications challenging. SyMGels are easily functionalised, using simple click-chemistry. This chemical flexibility, allows the creation of microenvironments with discrete biological decoration. Cellular control is demonstrated using MSC (mesenchymal stem cells)/chondrocytes and enables the regulation of key biomarkers such as aggrecan and SOX9. These potential therapeutic platforms demonstrate an important advancement in the biomaterial field, underpinning the mechanisms which drive their mechanical properties, and providing a versatile delivery system for advanced therapeutics.
Highlights
Introduction hindered large scale adoptionHydrogels have been regarded as an alternative for such materials, providing an ECM-like struc-The role of biomaterials within medicine and tissue engineer- ture to immobilise cells for transplantation.[9]
Synthetic microgel suspensions (SyMGels) were prepared using a shear-gel technique previously reported for polysaccharide based fluid gels;[12,21,31,39,40] whereby shear was applied to a polymer sol undergoing a sol-gel transition
One class of materials which, due to their unique material behaviors, have gained much attention are fluid gels. Like their quiescently gelled counterparts, possess all of the widelyreported advantages of hydrogels, yet they offer the ability to control the microstructure throughout the gelation process into a particulate suspension, which results in solid-like behavior at rest and liquid-like behavior on shearing.[25]
Summary
Introduction hindered large scale adoptionHydrogels have been regarded as an alternative for such materials, providing an ECM-like struc-The role of biomaterials within medicine and tissue engineer- ture to immobilise cells for transplantation.[9]. Hydrogels have been regarded as an alternative for such materials, providing an ECM-like struc-. The role of biomaterials within medicine and tissue engineer- ture to immobilise cells for transplantation.[9] Their tolerance ing has received growing attention within recent years, in biological environments, high-water content, mass transport their usage has been documented for millennia.[1] Scientific and and versatility have directly resulted in such materials becomtechnological advances have led to vast improvements within ing adopted into numerous tissue engineering and drug delivery applications.[10] translation of these new materials is. Moakes Healthcare Technologies Institute still slow, with large costs surrounding toxicology studies stemming from chemical, physical and morphological roles in modulating cellular events.[11]
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