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Self-assembly and elasticity of hierarchical proteoglycan–hyaluronan brushes† †Electronic supplementary information (ESI) available: Variations in areal mass density upon SLB and SAv monolayer formation determined by SE (Fig. S1). See DOI: 10.1039/c3sm51213d Click here for additional data file.

ABSTRACT: Spatially confined yet strongly hydrated assemblies made from the proteoglycan aggrecan and the polysaccharide hyaluronan (HA) are major, functionally important components of the pericellular space around chondrocytes, and in cartilage. To better understand, how mechanical properties arise from the supramolecular structure and dynamics of such assemblies, we have studied the effect of aggrecan on the physico-chemical properties of well-defined, planar HA brushes. From interaction studies by quartz crystal microbalance with dissipation monitoring and spectroscopic ellipsometry, and compression studies by combined colloidal probe atomic force/reflection interference contrast microscopy, we find that aggrecan readily intercalates into HA brushes in a reversible manner. Aggrecan induces a drastic swelling of HA brushes, generating self-assembled films of several micrometers in thickness that are highly hydrated (>99%), elastic and very soft. The Young modulus in the linear compression regime is well below 100 Pa, and reaches several kPa at strong compression. The implications of these findings for biological function are discussed.

SUBMITTER: Attili S

PROVIDER: S-EPMC4080815 | biostudies-other | 2013 Nov

REPOSITORIES: biostudies-other

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Project description:Thiol-ene 'click' chemistries have been widely used in biomaterials applications, including drug delivery, tissue engineering, and controlled cell culture, owing to their rapid, cytocompatible, and often orthogonal reactivity. In particular, hydrogel-based biomaterials formed by photoinitiated thiol-ene reactions afford spatiotemporal control over the biochemical and biomechanical properties of the network for creating synthetic materials that mimic the extracellular matrix or enable controlled drug release. However, the use of charged peptides functionalized with cysteines, which can form disulfides prior to reaction, and vinyl monomers that require multistep syntheses and contain ester bonds, may lead to undesired inhomogeneity or degradation under cell culture conditions. Here, we designed a thiol-ene hydrogel formed by the reaction of allyloxycarbonyl-functionalized peptides and thiol-functionalized poly(ethylene glycol). Hydrogels were polymerized by free radical initiation under cytocompatible doses of long wavelength ultraviolet light in the presence of water-soluble photoinitiators (lithium acylphosphinate, LAP, and 2-hydroxy-1-[4-(2-hydroxyethoxy)phenyl]-2-methyl-1-propanone, Irgacure 2959). Mechanical properties of these hydrogels were controlled by varying the monomer concentration to mimic a range of soft tissue environments, and hydrogel stability in cell culture medium was observed over weeks. Patterns of biochemical cues were created within the hydrogels post-formation and confirmed through the incorporation of fluorescently-labeled peptides and Ellman's assay to detect free thiols. Human mesenchymal stem cells remained viable after encapsulation and subsequent photopatterning, demonstrating the utility of the monomers and hydrogels for three-dimensional cell culture. This facile approach enables the formation and characterization of hydrogels with well-defined, spatially-specific properties and expands the suite of monomers available for three-dimensional cell culture and other biological applications.

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