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Intracellularly Degradable Hydrogen‐Bonded Polymer Capsules
Authors:Kristian Kempe  Sher Leen Ng  Sylvia T Gunawan  Ka Fung Noi  Frank Caruso
Affiliation:Department of Chemical and Biomolecular Engineering, The University of Melbourne, Victoria, Australia
Abstract:The assembly of low‐fouling polymer capsules with redox‐responsive behavior and intracellular degradability is reported. Thiol‐containing poly(2‐ethyl‐2‐oxazoline) (PEtOxMASH) brushes are synthesized by atom transfer radical polymerization (ATRP) of oligo(2‐ethyl‐2‐oxazoline)methacrylate and glycidyl methacrylate (GMA) and subsequent ring‐opening reaction of the GMA. Sequential deposition of PEtOxMASH/poly(methacrylic acid) (PMA) multilayers onto silica (SiO2) particle templates and crosslinking through disulfide formation yield stable capsules after the removal of the SiO2 templates by buffered hydrofluoric acid (HF). The redox‐responsive nature of the disulfide crosslinking groups enables the degradation of these capsules under simulated intracellular conditions at pH 5.9 and 5 mm glutathione (GSH). Furthermore, capsule degradation is observed after incubation with dendritic (JAWS II) cells. Even at high capsule‐to‐cell ratios, PEtOxMASH capsules show only negligible cytotoxicity. Quartz crystal microgravimetry (QCM) studies, using 100% human serum, reveal that films prepared from PEtOxMASH exhibit low‐fouling properties. The degradation and low‐fouling properties are promising for application of PEtOxMASH films/capsules for the delivery and triggered release of therapeutics.
Keywords:layer‐by‐layer  poly(2‐oxazoline)s  biofouling  degradation  disulfide bonds
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