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Injectable, self-healing hydrogels with enhanced solubilization of hydrophobic drugs are urgently needed for antimicrobial intravaginal therapies. Here, we report the first hydrogel systems constructed of dynamic boronic esters cross-linking unimolecular micelles, which are a reservoir of antifungal hydrophobic drug molecules. The selective hydrophobization of hyperbranched polyglycidol with phenyl units in the core via ester or urethane bonds enabled the solubilization of clotrimazole, a water-insoluble drug of broad antifungal properties. The encapsulation efficiency of clotrimazole increases with the degree of the HbPGL core modification; however, the encapsulation is more favorable in the case of urethane derivatives. In addition, the rate of clotrimazole release was lower from HbPGL hydrophobized via urethane bonds than with ester linkages. In this work, we also revealed that the hydrophobization degree of HbPGL significantly influences the rheological properties of its hydrogels with poly(acrylamide

Dynamic hydrogels with thermosensitive cross-links are highly promising platforms for "on-demand" drug delivery systems. However, there is a problem with triggering a response in their whole volume, which reduces their efficiency. To achieve better thermoresponsiveness, a graphene oxide-filled composite hydrogel based on boronic ester cross-links, composed of hyperbranched polyglycidol, HbPGL, and poly(acrylamide-ran-2-acrylamidephenylboronic acid), poly(AM-ran-2-AAPBA), has been constructed. The homogeneous embedment of graphene oxide (GO) in the network assured near-infrared (NIR)-photothermal response in its bulk due to the rapid light-to-heat conversion. The rate and amplitude of materials response increase with graphene oxide concentration. The temperature of the hydrogel containing graphene oxide at a concentration of 13.2 mg/mL increased from 36.6 to 41 °C in 29 s upon NIR irradiation. The network diffusivity and the extent of its change with temperature can be regulated by the length of the applied boronic acid-based cross-linking agent. The hydrogel constructed on the shorter copolymer (

We present biocompatible hydrogel systems suitable for biomineralization processes based on hyperbranched polyglycidol cross-linked with acrylamide copolymer bearing carbonyl-coordinated boronic acid. At neutral pH, diol functional groups of HbPGL react with boronic acid of polyacrylamide to generate 3D network in water by the formation of boronic ester cross-links. The dynamic associative/dissociative characteristics of the cross-links makes the network reversible. The presented hydrogels display self-healing properties and are injectable, facilitating gap filing of bone tissue. The 1H HR MAS DOSY NMR studies reveal that acrylamide copolymer plays the role of the network framework, whereas HbPGL macromolecules, due to their compact structure, move between reactive sites of the copolymer. The influence of the copolymer macromolecules entanglements and overall polymer concentrations on macromolecules mobility and stress relaxation processes is investigated. The process of hydrogel biomineralization results...