Gelation characteristics, physico-mechanical properties and degradation kinetics of micellar hydrogels

• PEG extended with aliphatic hydroxy acid (HA) segment to form degradable gels.
• The HA-chain-extended PEG was soluble in water and formed micellar structures.
• Micelle formation led to gels with tunable degradation from days to months.
• Micelle formation enhanced differentiation of mesenchymal stem cells in gels.

Due to their high water content and diffusivity of nutrients and biomolecules, hydrogels are very attractive as a matrix for growth factor immobilization and in situ delivery of cells to the site of regeneration in tissue engineering. The formation of micellar structures at the nanoscale in hydrogels alters the spatial distribution of the reactive groups and affects the rate and extent of crosslinking and mechanical properties of the hydrogel. Further, the degradation rate of a hydrogel is strongly affected by the proximity of water molecules to the hydrolytically degradable segments at the nanoscale. The objective of this review is to summarize the unique properties of micellar hydrogels with a focus on our previous work on star polyethylene glycol (PEG) macromonomers chain extended with short aliphatic hydroxy acid (HA) segments (SPEXA hydrogels). Micellar SPEXA hydrogels have faster gelation rates and higher compressive moduli compared to their non-micellar counterpart. Owing to their micellar structure, SPEXA hydrogels have a wide range of degradation rates from a few days to many months as opposed to non-degradable PEG gels while both gels possess similar water contents. Furthermore, the viability and differentiation of mesenchymal stem cells (MSCs) is enhanced when the cells are encapsulated in degradable micellar SPEXA gels compared with those cells encapsulated in non-micellar PEG gels.

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