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    Thermoresponsive Hydrogels Based on Telechelic Polyelectrolytes: From Dynamic to “Frozen” Networks

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    A novel thermoresponsive gelator of (B-<i>co</i>-C)-<i>b</i>-A-<i>b</i>-(B-<i>co</i>-C) topology, comprising a poly­(2-(dimethyl­amino)­ethyl methacrylate) (PDMAEMA) weak polyelectrolyte as central block, end-capped by thermosensitive poly­(triethylene glycol methyl ether methacrylate/<i>n</i>-butyl methacrylate) [P­(TEGMA-<i>co</i>-<i>n</i>BuMA)] random copolymers, was designed and explored in aqueous media. The main target of this design was to control the dynamics of the stickers by temperature as to create an injectable hydrogel that behaves as a weak gel at low temperature and as a strong gel at physiological temperature. Indeed, at low temperatures, the system behaves like a viscoelastic complex fluid (dynamic network), while at higher temperatures, an elastic hydrogel is formed (“frozen” network). The viscosity increases exponentially upon heating, about 5 orders of magnitude from 5 to 45 °C, which is attributed to the exponential increase of the lifetime of the self-assembled stickers. The integration of thermo- and shear responsive properties in the gelator endows the gel with injectability. Moreover, the gel can be rapidly recovered upon cessation of the applied stress at 37 °C, simulating conditions similar to those of injection through a 28-gauge syringe needle. All these hydrogel properties render it a good candidate for potential applications in cell transplantation through injection strategies