Structures and properties of hydrogels controlled by coordination bonds
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We developed hyaluronic acid (HA) hydrogels by regulating the gelation kinetics of Fe3+ and catechols, including Fe3+-induced covalent bonding and coordination bonding. Tetra-poly(ethylene glycol) with catechol end groups (t-PEG-CA) was also crosslinked through coordination bonds between catechol moieties and Fe3+, which produce bis-complex and tris-complex depending on pHs. The structures and properties of t-PEG-CA gels were examined upon the bonding types controlled by pHs and molar ratios between catechol groups and Fe3+. The correlation lengths (ξ) were determined in the solution regime and the t-PEG gel networks using light scattering, small-angle X-ray scattering, and neutron scattering measurements. For the gels with bis-complex units, ξ values correspond to the size of a single polymer chain. They increased in the gels consisting of tris-complex units, indicating that the matrices have partial crosslinks.