Direct-Ink Write 3D Printing Multistimuli-Responsive Hydrogels and Post-Functionalization Via Disulfide Exchange AITranslate

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DOI：https://doi.org/10.1021/acsapm.1c01538

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Herein, we describe a multistimuli-responsive hydrogel that can be 3D printed via a direct-ink write process to afford cross-linked hydrogel networks that can be postfunctionalized with thiol-bearing molecules. Poly(alkyl glycidyl ether)s with methacrylate groups at their termini were synthesized and self-assembled into hydrogels with three key stimuli-responsive behaviors necessary for extrusion-based 3D printing: a sol–gel temperature response, shear-thinning behavior, and the ability to be photochemically cross-linked. In addition, the chemically cross-linked hydrogels demonstrated a temperature-dependent swelling consistent with an LCST behavior. Pyridyl disulfide urethane methacrylate (PDS-UM) monomers were introduced into the network as a thiol-reactive handle for postfunctionalization of the hydrogel. The reactivities of these hydrogels were investigated at different temperatures (5, 25, and 37 °C) and swelling statuses (as-cured/preswollen) using glutathione as a reactive probe. To illustrate the versatility of the platform, we conjugated a number of additional thiol-containing probes such as proteins, polymers, and small molecules to the hydrogel network at different temperatures, pH values, and concentrations. In a final demonstration of the multistimuli-responsive hydrogel platform, a customized DIW 3D printer was used to fabricate a printed object that was subsequently conjugated with a fluorescent tag and displayed the ability to change in size with environmental temperature.