Tunable Drug Release from Supramolecular Hydrogels 3D-Printed by Visible-Light Reversible Addition–Fragmentation Chain Transfer Polymerization

Résumé fourni par la source

Abstract Precise control over drug release from 3D-printed hydrogels remains a central challenge in personalized medicine. Here, we report the integration of reversible addition–fragmentation chain transfer (RAFT) polymerization with supramolecular chemistry in a visible-light digital light processing (DLP) platform to fabricate customized, water-swellable, drug-loaded hydrogels with tunable release profiles. Using a reductive photoinduced electron transfer (PET)-RAFT mechanism under green light (λ = 528 nm), charged and hydrophilic monomers ([2-(acryloyloxy)ethyl]trimethylammonium chloride, TMAEA, and 1-vinyl-2-pyrrolidinone, NVP) were incorporated alongside poly(ethylene glycol) diacrylate (PEGDA) to yield covalently cross-linked networks capable of extensive swelling. By systematically varying the monomer-to-RAFT agent ratio, we demonstrate that RAFT concentration influences swelling and drug release through its effect on polymer growth and network formation. Among the formulations investigated, an intermediate RAFT concentration (monomer: RAFT = 500:1) exhibited the highest swelling ratio and near-complete release (97%) of the model drug paracetamol within 24 h. Deviations toward higher or lower RAFT concentrations resulted in reduced release of 73–82%. Swelling measurements, scanning electron microscopy, and gel permeation chromatography collectively support a model in which RAFT concentration modulates network formation, thereby influencing water accessibility and drug diffusion. This work establishes a design framework for tuning drug release from 3D-printed hydrogels through control of RAFT concentration and demonstrates visible-light PET-RAFT photopolymerization as a versatile, low-energy platform for personalized drug delivery.

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